Redmayne, currently head of commercial partnerships at Sky, will report to Victoria Barnsley, chief executive and publisher.
He is due to start the newly created role on Monday March 3 and will sit on the executive committee.
In his new role, Redmayne will be responsible for implementing a company-wide strategy to enhance existing digital income and exploit potential digital revenues by maximising HarperCollins content across multiple platforms and channels.
On a day-to-day basis he will oversee the group's digital publishing projects, including audio and ebooks, forming strategic partnerships with external digital and online contacts and leading new digital initiatives across the company.
Barnsley said: "HarperCollins is at the forefront of digital innovation and we are delighted to have secured someone of Charlie's impressive calibre and experience to head up our rapidly expanding digital programme."
Redmayne has racked up 18 years' experience in the advertising and online publishing industries.
He began his career in TV ad sales at TVAM and then Sky, before launching a media buying and sponsorship business called RCL Communications. RCL went on to launch Blink, the music based screen entertainment business, in 1996.
He left RCL in 2000 to launch the teen girl portal MyKindaPlace.com along with several other sites. Following the sale of MyKindaPlace to Sky in June 2006 he continued to run the business until last September, when he moved across to Sky full-time as head of commercial partnerships for its new online business unit.
Redmayne said: "The publishing industry is fast evolving into a multi-platform content delivery business. HarperCollins has already taken great strides in this direction.
"I believe there is an outstanding opportunity to harness the potential of both the online and mobile spaces to bring us closer to our customers, find new ways of marketing and distributing our content and increase our earnings potential."
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