Elsewhere in group A2, Rodrigo provided an assist of his own, as the City midfielder and his Spain colleagues secured a dramatic 2-2 draw away to the Czech Republic.
Cancelo was on target to round off what was a comprehensive win by Portugal in Lisbon against the Swiss.
The hosts had swept into a 3-0 lead by the break thanks to a brace from Cristiano Ronaldo and an effort by William Carvalho.
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And 22 minutes from time, Cancelo set the seal on a dominant display from the hosts by firing home a right foot shot from the edge of the box thanks to a fine assist from City colleague Bernardo Silva who had just come on as a substitute
Meanwhile, in the night’s other game in group A2, Rodri was a first half provider to help Spain earn a share of the spoils against the Czech Republic in Prague.
The hosts had taken an early lead with Jakub Pesek firing home on four minutes.
Luis Enrique’s side hit back to draw level in first half stoppage time with Barcelona’s Gavi side footing home from Rodri’s pinpoint assist.
The City midfielder came close to firing Spain ahead with a low drive just fizzing wide before he was taken off on the hour.
However, it was the Czech Republic who then struck again, Jan Kuchta hitting the target on 66 minutes.
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But Enrique’s side ensured the points were shared with Inigo Martinez heading home a dramatic equaliser in injury time.
The results left Portugal on top with four points from two games, just ahead of the Czechs on goal difference. Spain lie in third with two points and Switzerland bottom without a point so far.
The next games in A2 on Thursday see Portugal play host to the Czech Republic and Spain entertain Switzerland.