The two crossword solutions for the term 'Largest Country in Africa' are Sudan (5 letters) and ALGERIA (7 letters). Sudan is a country located in Northeast Africa, bordered by Egypt to the north, the Red Sea to the northeast, Eritrea and Ethiopia to the east, South Sudan to the south, the Central African Republic to the southwest, Chad to the west, and Libya to the northwest. ALGERIA is a country located in North Africa, bordered by Tunisia to the northeast, Libya to the east, Niger to the southeast, Mali and Mauritania to the southwest, Morocco to the west, and the Mediterranean Sea to the north. Both Sudan and ALGERIA are large countries in Africa, with Sudan being the largest in terms of land area and ALGERIA being the largest in terms of population.