Djokovic, the world number two, earned the decisive point by beating Marin Cilic 6-3, 6-3, 6-2.
"On Friday and today Novak Djokovic was an unbridgeable obstacle, he played great tennis," Croatia coach Goran Prpic said.
"We all wanted and were hoping to win this match but we have to admit that (Serbia) they were better," he added.
Djokovic did not offer his opponent any chance and built up a 5-0 lead in the first set to give an early hint at the outcome of the match. The other two sets had a similar scenario paving the way for the Serb's final triumph over an uncertain Cilic.
In the opening match of the tie between the former Balkan foes on Friday Djokovic beat Croatia's Ivan Ljubicic 7-6 (7/3), 6-4, 6-1, and Cilic saw off Serb Viktor Troicki 6-4, 7-5, 6-2.
Serbia moved closer to a Davis Cup semifinal berth after their doubles duo Nenad Zimonjic and Janko Tipsarevic beat their Croatian opponents on Saturday.
Zimonjic and Tipsarevic beat Cilic and Ivan Dodig 6-3, 6-2, 6-4 in just under two hours in the third of the best-of-five rubbers in the coastal town of Split.
Croatia won the Davis Cup in 2005 and reached the semifinal last year.
In its first semifinal ever Serbia is to play against the Czech Republic at home.
The final dead rubber on Sunday will see Croat Antonio Veic facing Tipsarevic.
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