The 455-mile journey will connect 22 stations between the capitals of Wales and Scotland directly by rail.
Passengers are already able to book journeys on the new route.
Scott Maynard, CrossCountry’s Interim Managing Director, said: “We’re delighted to introduce this new service joining Cardiff and Edinburgh directly by rail for the very first time – meaning even more connections for customers across the length and breadth of the country.
“Thanks to colleagues across CrossCountry and the wider rail industry for their support in delivering these new services linking two of Great Britain’s capital cities, as well as many other key towns and cities in between.”
The new service will be formed by long-distance Voyager services departing from Cardiff and Penzance in the morning, joining together at Birmingham New Street before proceeding north to Edinburgh.
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On the southbound journey, the long-distance Voyager train will depart from Edinburgh and proceed to Gloucester where the service splits into two. Half of the train will travel onwards to Cardiff whilst the other half will terminate at Plymouth.
There will be one service in each direction between Cardiff and Edinburgh on weekdays only.
Scotland’s Cabinet Secretary for Transport, Fiona Hyslop added: “The launch of a new direct weekday train service between Edinburgh and Cardiff for the first time is welcome news for rail users wishing to travel between these two capital cities.
“The new service should have a positive impact for jobs and local economic growth, while providing direct connectivity between Scotland, Wales, and intermediary locations when it commences later this year.”
Wales’ Cabinet Secretary for Transport and North Wales, Ken Skates, said: “We are always happy to support new services that offer more choice for passengers. Connecting two capital cities of the UK in a sustainable way is a positive development.”