Having only been in the post for two months, the former MP for Portsmouth South said she was leaving the post "to avoid any disruption to the work of the PCC and his staff".
The youth and community development charity Active Communities Network has secured Home Office funding to run a number of workshops in the Portsmouth and Havant areas.
The aim of the Cyber Ambassador scheme is to enable skilled-up, informed pupils to educate and offer advice and support to their peers so they can make the most of the internet and stay safe.