The first phase of the three-year partnership will start in January in Bury, Leeds, Merseyside and Slough.
A group of 80 young people aged 16 to 17 have already been recruited and will be trained to provide peer-mentoring support in their schools.
They will be supported by 80 employees from O2 who will be trained to provide dedicated one-to-one support such as motivation and engagement.
O2 employees also intend to raise up to 1m for the young people's charity through fundraising over three years.
A Weston Spirit spokeswoman said: "O2's employees will add another layer of support to the young peer mentors, and will learn mentoring skills that will benefit their own organisation too."
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