He was part of one of the best Portuguesa teams of all time, where alongside players like Pinga, Julinho Botelho and Brandãozinho he won the Rio-São Paulo Tournament in 1952 and 1955 and the Blue Ribbon in 1951 and 1953.

He was featured in the first academy alongside stars such as Ademir da Guia, Julinho Botelho, Djalma Dias and Vavá.

Despite having only defended three clubs in his career, Djalma Santos once wore the jersey of São Paulo, even though he belonged to Palmeiras at the time.

On 9 November 1960, he played as an honor guest in the celebrations of the inauguration of the Morumbi Stadium, in the victory over Nacional do Uruguay, by 3–0, with goals from Canhoteiro and Gino.

[4] Santos made his World Cup debut in a 5–0 win against Mexico, and played in all of Brazil's matches during the tournament.

Noting that the Slovak goalkeeper Viliam Schrojf was somewhat off his line, Santos lofted a long, massive, high arcing ball, into the goalmouth aided by the glare of the afternoon sun.

After beginning his career in midfield, Santos found much success as a defender due to his composure, as well as his excellent and consistent displays in this position, and is regarded as one of the greatest right-backs of all time; he was also capable of playing as a centre back.

[6] Santos was a quick and physically strong defender, who was known for his stamina, marking, and tackling ability; he was also effective in the air.

[2][3] In addition to his defensive ability as a right-back, which earned him the nickname Muralha (the wall) from the Uruguayan writer Eduardo Galeano, Santos was also known for his excellent technique and offensive capabilities, which saw him contribute to the development of the role; being gifted with excellent ball control, good dribbling skills, creativity, and accurate distribution, he often took on opponents with the ball when under pressure in one on one situations, even in risky situations inside his own penalty area, and he was also one of the first full-backs to venture forward and make overlapping attacking runs down the flank in order to contribute to his teams' offensive plays.