Northern Ireland and Scotland have pledged to work together on tourism, education, renewable energy and strengthening cultural ties.
Scottish First Minister Alex Salmond and his NI counterparts, Ian Paisley and Martin McGuinness, signed the agreement at Stormont.
Mr Salmond said his visit to Northern Ireland had exceeded expectations.
He also revealed that Mr Paisley and Mr McGuinness will make a reciprocal visit to Edinburgh in the autumn.
"We have made progress across a number of areas," the Scottish first minister said.
"This has been a very useful trip which has exceeded our expectations. We are now going to get down to the nitty gritty of working together on issues like education, transport, tourism, and we will also be working with Wales.
"I think there is a realisation that this is a far better way for the devolved administrations to do business.
"Given the series of misunderstandings that have existed between Scotland and Westminster and Wales and Westminster, we are arguing that the resurrection of joint-ministerial committees involving the three devolved administrations and the government in London is a good way forward.
"I also believe the next prime minister will also prefer this way of decision-making."
Mr Salmond also agreed to look at the possibility of Northern Ireland students attending universities in Scotland benefiting from his executive's decision last week to scrap the £2,000 endowment fee paid after graduation.
The two devolved governments will also look at building links between universities and colleges, and ferry links, including the summer service between Campbeltown on the west coast of Scotland and Ballycastle, County Antrim.