DropDownList ddl = new DropDownList();

ddl.DataSource = GetCountries;
ddl.DataBind();

OR USE
foreach (string name in GetCountries){
ddl.Items.Add(new ListItem(name.ToString()));
}

List<string> GetCountries() {
List<string> countries = new List<string>();
countries.Add("Afghanistan");
countries.Add("Aland Islands");
countries.Add("Albania");
countries.Add("Algeria");
countries.Add("American Samoa");
countries.Add("Andorra");
countries.Add("Angola");
countries.Add("Anguilla");
countries.Add("Antarctica");
countries.Add("Antigua and Barbuda");
countries.Add("Argentina");
countries.Add("Armenia");
countries.Add("Aruba");
countries.Add("Australia");
countries.Add("Austria");
countries.Add("Azerbaijan");
countries.Add("Bahamas");
countries.Add("Bahrain");
countries.Add("Bangladesh");
countries.Add("Barbados");
countries.Add("Belarus");
countries.Add("Belgium");
countries.Add("Belize");
countries.Add("Benin");
countries.Add("Bermuda");
countries.Add("Bhutan");
countries.Add("Bolivia");
countries.Add("Bosnia and Herzegovina");
countries.Add("Botswana");
countries.Add("Bouvet Island");
countries.Add("Brazil");
countries.Add("British Indian Ocean Territory");
countries.Add("Brunei");
countries.Add("Bulgaria");
countries.Add("Burkina Faso");
countries.Add("Burundi");
countries.Add("Cambodia");
countries.Add("Cameroon");
countries.Add("Canada");
countries.Add("Cape Verde");
countries.Add("Cayman Islands");
countries.Add("Central African Republic");
countries.Add("Chad");
countries.Add("Chile");
countries.Add("China");
countries.Add("Christmas Island");
countries.Add("Cocos Islands");
countries.Add("Colombia");
countries.Add("Comoros");
countries.Add("Congo");
countries.Add("Congo, Democratic Republic of the");
countries.Add("Cook Islands");
countries.Add("Costa Rica");
countries.Add("Côte d&#39;Ivoire");
countries.Add("Croatia");
countries.Add("Cuba");
countries.Add("Cyprus");
countries.Add("Czech Republic");
countries.Add("Denmark");
countries.Add("Djibouti");
countries.Add("Dominica");
countries.Add("Dominican Republic");
countries.Add("East Timor");
countries.Add("Ecuador");
countries.Add("Egypt");
countries.Add("El Salvador");
countries.Add("Equatorial Guinea");
countries.Add("Eritrea");
countries.Add("Estonia");
countries.Add("Ethiopia");
countries.Add("Falkland Islands");
countries.Add("Faroe Islands");
countries.Add("Fiji");
countries.Add("Finland");
countries.Add("France");
countries.Add("French Guiana");
countries.Add("French Polynesia");
countries.Add("French Southern Territories");
countries.Add("Gabon");
countries.Add("Gambia");
countries.Add("Georgia");
countries.Add("Germany");
countries.Add("Ghana");
countries.Add("Gibraltar");
countries.Add("Greece");
countries.Add("Greenland");
countries.Add("Grenada");
countries.Add("Guadeloupe");
countries.Add("Guam");
countries.Add("Guatemala");
countries.Add("Guernsey");
countries.Add("Guinea");
countries.Add("Guinea-Bissau");
countries.Add("Guyana");
countries.Add("Haiti");
countries.Add("Heard Island and McDonald Islands");
countries.Add("Honduras");
countries.Add("Hong Kong");
countries.Add("Hungary");
countries.Add("Iceland");
countries.Add("India");
countries.Add("Indonesia");
countries.Add("Iran");
countries.Add("Iraq");
countries.Add("Ireland");
countries.Add("Isle of Man");
countries.Add("Israel");
countries.Add("Italy");
countries.Add("Jamaica");
countries.Add("Japan");
countries.Add("Jersey");
countries.Add("Jordan");
countries.Add("Kazakhstan");
countries.Add("Kenya");
countries.Add("Kiribati");
countries.Add("Kuwait");
countries.Add("Kyrgyzstan");
countries.Add("Laos");
countries.Add("Latvia");
countries.Add("Lebanon");
countries.Add("Lesotho");
countries.Add("Liberia");
countries.Add("Libya");
countries.Add("Liechtenstein");
countries.Add("Lithuania");
countries.Add("Luxembourg");
countries.Add("Macao");
countries.Add("Macedonia");
countries.Add("Madagascar");
countries.Add("Malawi");
countries.Add("Malaysia");
countries.Add("Maldives");
countries.Add("Mali");
countries.Add("Malta");
countries.Add("Marshall Islands");
countries.Add("Martinique");
countries.Add("Mauritania");
countries.Add("Mauritius");
countries.Add("Mayotte");
countries.Add("Mexico");
countries.Add("Micronesia");
countries.Add("Moldova");
countries.Add("Monaco");
countries.Add("Mongolia");
countries.Add("Montenegro");
countries.Add("Montserrat");
countries.Add("Morocco");
countries.Add("Mozambique");
countries.Add("Myanmar");
countries.Add("Namibia");
countries.Add("Nauru");
countries.Add("Nepal");
countries.Add("Netherlands");
countries.Add("Netherlands Antilles");
countries.Add("New Caledonia");
countries.Add("New Zealand");
countries.Add("Nicaragua");
countries.Add("Niger");
countries.Add("Nigeria");
countries.Add("Niue");
countries.Add("Norfolk Island");
countries.Add("Northern Mariana Islands");
countries.Add("North Korea");
countries.Add("Norway");
countries.Add("Oman");
countries.Add("Pakistan");
countries.Add("Palau");
countries.Add("Palestine");
countries.Add("Panama");
countries.Add("Papua New Guinea");
countries.Add("Paraguay");
countries.Add("Peru");
countries.Add("Philippines");
countries.Add("Pitcairn");
countries.Add("Poland");
countries.Add("Portugal");
countries.Add("Puerto Rico");
countries.Add("Qatar");
countries.Add("Reunion");
countries.Add("Romania");
countries.Add("Russia");
countries.Add("Rwanda");
countries.Add("Saint Helena");
countries.Add("Saint Kitts and Nevis");
countries.Add("Saint Lucia");
countries.Add("Saint Pierre and Miquelon");
countries.Add("Saint Vincent and the Grenadines");
countries.Add("Samoa");
countries.Add("San Marino");
countries.Add("São Tomé and Príncipe");
countries.Add("Saudi Arabia");
countries.Add("Senegal");
countries.Add("Serbia");
countries.Add("Serbia and Montenegro");
countries.Add("Seychelles");
countries.Add("Sierra Leone");
countries.Add("Singapore");
countries.Add("Slovakia");
countries.Add("Slovenia");
countries.Add("Solomon Islands");
countries.Add("Somalia");
countries.Add("South Africa");
countries.Add("South Georgia and the South Sandwich Islands");
countries.Add("South Korea");
countries.Add("Spain");
countries.Add("Sri Lanka");
countries.Add("Sudan");
countries.Add("Suriname");
countries.Add("Svalbard and Jan Mayen");
countries.Add("Swaziland");
countries.Add("Sweden");
countries.Add("Switzerland");
countries.Add("Syria");
countries.Add("Taiwan");
countries.Add("Tajikistan");
countries.Add("Tanzania");
countries.Add("Thailand");
countries.Add("Togo");
countries.Add("Tokelau");
countries.Add("Tonga");
countries.Add("Trinidad and Tobago");
countries.Add("Tunisia");
countries.Add("Turkey");
countries.Add("Turkmenistan");
 countries.Add("Turks and Caicos Islands");
countries.Add("Tuvalu");
countries.Add("Uganda");
countries.Add("Ukraine");
countries.Add("United Arab Emirates");
countries.Add("United Kingdom");
countries.Add("United States");
countries.Add("United States minor outlying islands");
countries.Add("Uruguay");
countries.Add("Uzbekistan");
countries.Add("Vanuatu");
countries.Add("Vatican City");
countries.Add("Venezuela");
countries.Add("Vietnam");
countries.Add("Virgin Islands, British");
countries.Add("Virgin Islands, U.S.");
countries.Add("Wallis and Futuna");
countries.Add("Western Sahara");
countries.Add("Yemen");
countries.Add("Zambia");
countries.Add("Zimbabwe");
return countries;
}