Sharpedo's first major appearance was in Sharpedo Attack!. A pod of Sharpedo attacked Ash and his friends, plus Mr. Briney, while they were at an uncharted, crescent-shaped island. They gained the pod's trust when Brock healed their leader's injury when it came across Team Rocket.
Multiple Sharpedo appeared in PK13, where they were attacking Pikachu and the others to across the deserted island, where Aggron ties Azumarill.
A group of Sharpedo were used by J's henchmen to attack Ash and his friends, along with Kellyn, in Pokémon Ranger and the Kidnapped Riolu! Part One.