Benfica competed domestically in the Primeira Divisão and the Taça de Portugal and participated in the European Cup after winning the previous league.

They won three-nil at home and drew one-all in Vienna, qualifying for the European Cup final, where they would meet favourites Barcelona.

[8] In April, Benfica wrapped up the league, after drawing with Sporting CP on match-day 22, keeping a five-point lead.

[10] Qualified for the European Cup final, they would face favourites FC Barcelona, who had eliminated five-time winners and title-holders Real Madrid.

In the next minute, José Neto set up a long ball for Santana, with Barcelona defender, Enric Gensana heading it backwards into his own goal.

[11] In the second half, Cavém crossed another ball from the left, reaching Coluna, who waited at the front of the box, to score the 3–1.

[13] The season final game was with Belenenses in which Benfica won, therefore ending the league with a four-point lead over Sporting and 13 over Porto.

Note 2: Players with squad numbers marked ‡ joined the club during the 1960-61 season via transfer, with more details in the following section.