Tusk was greeted by Prime Minister Theresa May outside 10 Downing Street in London ahead of the bilateral meeting.
The talks come as both sides are settling on their negotiating positions. The European Parliament on Wednesday backed the bloc's chief negotiator in demanding Britain pay as much as 60 billion euros (USD 64 billion) for outstanding commitments.
EU lawmakers also called for phased negotiations, in which divorce terms are settled before a new trade deal is secured. Britain wants the two strands to go hand-in-hand.
Brexit talks are expected to start in late May once the negotiating guidelines of the EU's 27 remaining nations have been sealed in a mandate for EU chief negotiator Michel Barnier.
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