The Santos team of the 1962 and 1963 seasons is regarded as one of the best in South American football history, and it is regarded as the pinnacle of renowned striker Pele's club career. The team won the Libertadores and Intercontinental Cup back-to-back, defeating Benfica and AC Milan in the process. In the 1960s, no other team in Brazilian football enjoyed the same level of domination as Santos. Hundreds of specialists from South America and Europe voted the Santos team of 1962/63 as the best team of all time in a survey published in the magazine El Grafico.

Coach: Lula

Trophies: 2 Copa Libertadores (1962,1963), 2 Intercontinental Cups (1962,1963), 2 Brasileiro Série A (1962,1963), 1 Torneio Rio-São Paulo (1963), 1 Campeonato Paulista (1962)

Star Players: Pele, Zito, Pepe, Gilmar Coutinho

Santos were not one of Brazil's top clubs when Pele joined them, and their Vila Belmiro stadium barely held 25,000 people, but with him, they became two-time South American champions and then twice global winners. They answered any potential disputes regarding the relative strengths of South American football by defeating two famous Benfica and AC Milan sides over two legs, notably a 5-2 away win over Benfica in 1962. Of doubt, Pele played an important role on this team, but it was not a one-man show. He was supported in the attack by Pepe and his Brazil international teammates Zito and Gilmar.

Winners of the Serie A, Santos faced Penarol in the Copa Libertadores final. Winners on two occasions, Penarol was in their third final in a row, while Santos was looking to win the competition for the first time. The finals were split into two parts: home and away match. After the two legs, the team with the most points, two for a victory, one for a tie, and zero for a loss, would be proclaimed champion. Santos ended the Carboneros' hegemony in Buenos Aires, defeating Penarol 0-3 in the deciding playoff. For the first time, Santos was crowned South American champions and qualified for the 1962 Intercontinental Cup.

The 1962 Intercontinental Cup was a two-legged football match between Brazilian team Santos, the 1962 Copa Libertadores winners, and Portuguese club Benfica, the 1961–62 European Cup winners. For the first time, Santos had won the Intercontinental Cup. The match is famous for pitting Pelé of Brazil against Eusébio of Portugal, two of the best players of the 1960s who only met three times. Santos won the opening leg with a score of 3-2. The second leg, Santos' 2–5 win in Lisbon, in which Pelé scored a hat-trick, is widely regarded as the best performance in the competition's history.

Santos defended their Serie A once again in the following season and reached the finals of Copa Libertadores again. Santos, the defending champions, were in their second final in a row, while Boca Juniors were looking to win the championship for the first time. The Alvinegro da Vila, widely regarded as the best football club team ever, thrashed its semifinal and final opponents in spectacular fashion, including a 0–4 triumph over Botafogo at the legendary Estádio do Maracana and a 1–2 victory over Boca Juniors at La Bombonera. Santos overcame the Xeneixes on both legs of the final to retain their title in a classic South American match-up.

The 1963 Intercontinental Cup was played between Milan, the European Cup champions in 1962–63, and Santos, the Copa Libertadores champions in 1963. The tournament was in its fourth year. On October 16, 1963, the opening leg was held at the San Siro in Milan. Milan won the match 4–2 at home. The return leg was conducted at the Maracana in Rio de Janeiro the next month, on November 14th. The two clubs were tied on points after Santos won the match 4–2. As a result, a playoff was required two days later, which Santos won 1–0, ensuring the trophy.