But, on arriving in Lisbon at the age of 19, he was snatched by rival club Benfica for a fee of £7,500.
In one of his first games for the club, Eusebio scored a hat-trick against Santos, a side that included Brazilian star Pele, and confirmed his status as one of Europe's most lethal strikers.
The following year, he was a member of the first side to beat Real Madrid in a European Cup final when Benfica triumphed 5-3.
He won 10 league championships, five cups and one European Cup in his 15 years at Benfica and was Portugal's top league scorer between 1964 and 1973.
His dazzling tally of goals for club and country earned him the prestigious European Footballer of the Year award in 1965.
But it was a year later that he secured a new following with his performance in the World Cup in England.
After winning all their group games and helping to eliminate title-holders Brazil in the first round, newcomers Portugal came from 3-0 down to beat North Korea 5-3 in a dramatic quarter-final, thanks to four goals from Eusebio.
Portugal went on to lose 2-1 in the next round to eventual winners England and a tearful Eusebio left the pitch.
By then, he had captured the hearts of the British public and his figure was soon added to Madame Tussaud's waxwork collection.
Eusebio continued to play at the highest level until 1974, but knee problems had already begun to slow him down.
In 1975, he moved to the North American Soccer League and then returned to Portugal in 1976/77 to play for SC Beira Mar before further spells in the USA and Mexico.