With a landmark post-Brexit EU-UK summit due next month, both sides are seeking to improve ties amid the global turmoil ushered in by US President Donald Trump.
But Starmer faces a tricky balancing act, as he is also looking to reach out to the Trump administration and secure a favourable trade deal with the United States.
UK and EU officials have been hoping a defence and security pact will be the highlight of the May 19 meeting, as Trump's return to the White House casts doubt on the United States' commitment to NATO and European security.
Before Thursday's talks, European Commission President von der Leyen said the discussions with Starmer could lead to the UK joining a European defence programme.
"We will discuss work on a strategic security and defence partnership agreement, which might pave the way then to a joint procurement and UK participation in our SAFE programme," she said.
She was referring to a 150-billion-euro ($170-billion) joint EU fund allowing countries to buy missiles, artillery, drones, ammunition and other equipment.
Britain needs to sign a defence pact to be included in the fund, which could benefit UK companies including BAE Systems and Rolls Royce.
- Post-Brexit 'reset' -
The London summit in May is also meant to turn the page on years of post-Brexit strife, as part of a "reset" in relations promised by Starmer.
Welcoming von der Leyen to his Downing Street office after the pair attended a global energy security summit in London, Starmer said: "In a world which seems increasingly unstable with an uncertain future, it is so good that we are working so closely together on so many issues."
Following the talks, a Downing Street spokesperson said the pair made "good progress", without giving details on the defence pact.
The discussions "focused on a range of issues including Ukraine, energy security, the global economy and defence," the spokesperson said.
Von der Leyen posted on X that there was "great potential for more cooperation" on energy, migration, and "a dedicated partnership" on defence and security.
May's summit is set to be a milestone in Labour leader Starmer's pursuit of closer relations with the bloc following Britain's bitter 2020 departure under the previous Conservative government.
However Starmer has laid out strict red lines, while the EU has its own demands, raising questions about what exactly the talks can achieve.
Starmer has vowed Britain will not return to the single market or customs union and has ruled out signing up to freedom of movement across EU-UK borders.
lcm/rlp
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