The move will see the South Korean technology giant launch branded standalone stores showcasing its full range of mobiles, tablet computers and laptops in seven European markets within the next three months.
Carphone has been chosen as Samsung's "preferred partner" to launch and run the stores in Europe under a five-year contract, which follows a successful trial with three stores that opened in Spain last autumn.
Around 20 of the stores will open in the UK, with the remainder launching across Ireland, Germany, Spain, Portugal, Sweden and the Netherlands.
It will see Samsung step up the pressure on Apple, which already has a successful global retail store portfolio.
Samsung, which overtook Apple as the biggest smartphone seller in 2011, said the deal will create a "powerful new retail concept".
It is also said to be planning to open standalone stores across the US, reportedly hiring former Apple Store designer Tim Gudgel as part of the push.
The group already has Samsung Experience stores in the US as concessions within consumer electronics giant Best Buy, while it recently opened a Samsung Experience site in Westfield shopping centre in Stratford, London.
It also has a successful franchise chain in Thailand, but said the move into Europe is its first major roll out of standalone shops.
The stores planned with Carphone Warehouse will focus specifically on its mobile products and not its range of TVs and white goods, such as fridges, washing machines and vacuum cleaners.
It is hoped more stores could be launched across Europe under the deal.
Shares in Carphone raced 8% higher after the tie-up was announced.
Carphone already runs around 2,000 retail stores throughout Europe under the Carphone Warehouse and Phone House brands.
But the Samsung deal is not the first time it has joined forces with other firms to help them expand retail presences, having previously launched an ill-fated venture with US consumer electronics group Best Buy.
It placed its store estate into the joint venture in 2008, but bought Best Buy out last August as the US firm retrenched amid tough retail conditions in Europe.