The Real Madrid midfielder was clearly disappointed as Spain ran out 5-4 winners on penalties with the two sides playing out a dull goalless draw after 120 minutes of football.
Modric did his bit in the shootout as he converted his spot-kick but the contest was decided when Real Madrid teammate Dani Carvajal dinked his effort into the net after Bruno Petkovic had his shot saved by Unai Simon.
Modric has suffered worse heartache having been part of the Croatia side that lost the 2018 World Cup final to France, but at 37 years old, this could be his last chance to win a trophy at international level.
The result also meant that Croatia missed arguably their best chance of winning the first major trophy in the country's history.
There were no tears for Modric but a number of fans were quick to express their sadness at the legend not getting the silverware they feel he deserves.
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One fan tweeted: "No Luka Modric international trophy pics, football is unfair."
Another said: "Spanish or not, we all wanted to see Luka Modric finally win and lift a trophy with Croatia."
This one said: "I actually feel so so bad for Luka Modric man, the Croatia attack will not see the gates of heaven for their crimes."
And this fan said: "I feel so bad for Luka Modric man always carries his country every tournament just to let down by others."
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