The London-based print management group won the deal following a competitive tender process.
The three-year contract has an option to be extended for a further two years.
A Williams Lea team will be based on-site at Capital One's Nottingham headquarters, providing support to the firm's design and print teams.
Under the terms of the deal, the firm will handle design, including brand and content management, print procurement, including customer correspondence, security print and statements as well as document composition and postage.
All marketing-based print, such as brochure and direct mail, will be outsourced through Williams Lea's preferred vendors.
Unspecified elements of transactional print will be handled by Williams Lea, with the remainder also outsourced.
Financial services provider Capital One said it had been looking for a partner to develop a long-term relationship with, to improve its customer service and deliver substantial cost benefits.
Williams Lea's clients include Norwich Union, O2, BMW, Prudential, AXA, Merrill Lynch and Debenhams.
Williams Lea wins Capital One job
Williams Lea has secured a multi-million pound three-year contract to handle the design, print and distribution for Capital Ones transactional mail.