The Nigeria stars found the back of the net in the fiercely contested match which saw the hosts come out victorious at Stadio Diego Armando Maradona
Simeon Nwankwo scored a brace in Saturday's Serie A match but it was not enough as Victor Osimhen's goal helped Napoli beat Crotone 4-3.
The defeat was Crotone's 22nd league defeat this season but Simy's contributions at the Stadio Diego Armando Maradona took his tally to 15 goals after 29 league matches so far.
Osimhen, meanwhile, scored his fourth Serie A goal of the season by making it 2-0 for Gennaro Gattuso's side, three minutes after Lorenzo Insigne opened the scoring in the 19th minute.
Shortly after, Libya midfielder Ahmed Benali provided the assist for Simy to reduce the deficit for Crotone in the 25th minute but Dries Mertens restored Napoli's two-goal lead in the 34th minute.
Three minutes after the restart, Simy found the back of the net again and Junior Messias scored the equaliser for the visitors in the 59th minute.
With Crotone hoping to pick up their first point since their 4-2 win over Torino on March 7, Giovanni Di Lorenzo's 72nd-minute winner dealt a blow to them as Gattuso's men remain unbeaten in their last six matches.
Crotone are still rooted to the bottom of the Serie A table following the defeat with 15 points after 28 matches while Napoli are in fifth spot with 53 points from 27 outings.
Simy has scored eight goals in his last five matches for the Pythagoreans and he will be aiming to continue his rich vein of form when they travel to Spezia on April 10.
Osimhen, on the other hand, will hope to build on his second Serie A goal of the year when Napoli visit Juventus for a league match on Wednesday.
Osimhen recently returned from international duty with Nigeria where he scored a goal in the Super Eagles' 3-0 win over Lesotho in an Africa Cup of Nations qualifiers on Tuesday. Simy, however, was not included in Gernot Rohr's 24-man squad for the two games against Benin and the Crocodiles.