Although Spain dominated possession and pinned Morocco back for long portions of 120-plus minutes of regulation and extra time, the game ended 0-0 and went to penalties, where Spain had two attempts saved by Yassine Bounou and one come off the post before Achraf Hakimi netted the winning spot kick for the African side.
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"The responsibility is mine," Enrique said after the match. "I chose the first three penalty takers, who were those I thought were the best specialists on the pitch. We didn't even get to the fourth. Bounou is a spectacular goalkeeper in this aspect; he has a high percentage in going the right way. He was great."
It was the second time in as many World Cups that Spain were eliminated in a shootout -- losing to hosts Russia from the spot in 2018 -- and the former Barcelona manager was left to lament his team's inability to make their massive edge in possession count.
"Football is a marvelous, passionate sport, but a team can win without attacking," Luis Enrique said. "Morocco attacked once or twice and were dangerous, but we dominated the game completely, and tried to create."
The Spaniards completed 988 of 1,063 passes to 238 of 331 for the Moroccans and had 63% to 21% advantage in possession.
"We would have liked to create more. It was hard for us," added Luis Enrique. "We had 11 shots, I think, but few on goal. In the final move of the game Pablo Sarabia hit the post. The penalty shootout was hard for us. But I'm proud of my players."
Spain had the third-youngest squad at the World Cup, with Gavi, 18, and Pedri, who turned 20 during the tournament, showing maturity beyond their years at the heart of the team's midfield, while 20-year-old strikers Ansu Fati and Nico Williams looked full of potential when they came off the bench.
However, the Spain coach was frank in his final assessment of the outcome, while also addressing his future as manager of the national team.
"We have to congratulate the winners," Luis Enrique said. "They played their game, it turned out well, they were better than us in the penalty shootout. I think children have to learn how to lose, regardless of whether you deserve it or not.
"Right now I'm looking forward to getting home to see my family and my dogs and be with them. I suppose that from next week, when the president [Luis Rubiales] considers it timely, we'll talk about what the future can bring. Right now that means nothing to me, because we need to assimilate this disappointment and deal with it in the best way."
Veteran Spain midfielder Sergio Busquets also speculated on what might have been following the loss and said that deciding a match from the penalty spot was always a 50-50 proposition after seeing one of his spot kicks denied by Bounou.
"We wanted to continue [in the competition]," Busquets said. "I think we did well, it was a tough, physical game; as time passed we found more spaces, and in extra time it was the same. We even had Sarabia's chance, which was a shame, and then it was penalties in the cruelest way.
"It was hard for us. We tried to tire them out, to find spaces. Sometimes we managed it, and we lacked a bit of luck, the final ball or the finish.
"It's always heads or tails [with penalties]. We missed the first three penalties and it's very difficult like that."
Spain, which won the World Cup in 2010, have now failed to reach the quarterfinals in four of their past five appearances.