The win marks the second Nations League for Portugal after lifting the inaugural edition's trophy in 2019.
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Portugal defeated Spain in penalty kicks 5- 3 to win the UEFA Nations League final late on Sunday after both sides failed to score in extra time following a showdown that ended 2-2.
After Nuno Mendes, Bruno Fernandes, Vitinha, and Goncalo Ramos all smoothly scored their penalties, Portugal goalkeeper Diogo Costa saved Spain's Álvaro Morata’s spot kick before Neves converted his team’s fifth to seal the win.
The win marks the second Nations League trophy for Portugal after lifting the inaugural edition in 2019.
Its victory against Spain, the reigning European champions, was hard-fought, as the Seleção had come back twice from behind.
Cristiano Ronaldo sent the match to extra time when he equalised in the 61st minute with his record-extending 138th goal for Portugal.
The 40-year-old Ronaldo went off to a standing ovation and a hug from coach Roberto Martínez in the 88th.
The keenly contested final seemed destined for Spain after Mikel Oyarzabal had given Spain a 2-1 halftime lead. Oyarzabal squeezed the ball past Portugal goalkeeper Diogo Costa in the 45th minute after Pedri played him through on goal.
It was also Spain who drew the first blood after Martin Zubimendi broke the deadlock in the 21st minute with a tap-in when Portugal’s defence failed to deal with Lamine Yamal’s cross.
Five minutes later, Portugal responded with Nuno Mendes levelling by drilling a low shot inside the far post.
Lamine Yamal, the Spanish sensation and favourite to win the Ballon d'Or, was mostly marked out of the game by Portugal full-back Mendes, ensuring Yamal could pose no major threat before being subbed off in extra time.
Les Bleus get Third place
Earlier on Sunday, Kylian Mbappé led France to defeat host Germany 2-0 in Stuttgart, securing third place.
The Real Madrid forward helped Les Bleus bounce back from a sluggish first half by scoring one goal and setting up another for Michael Olise.
The goal was Mbappe's 50th for France in international competition.