The two met on the sidelines of a summit with European leaders as London looks to reset its relationship with the EU and turn the page on rocky post-Brexit relations.
"Looking to the future, France and the UK will pursue their cooperation across the full spectrum of the relationship," they said in a joint statement.
The two leaders also addressed the issue of migrants crossing the Channel from France to Britain, a sensitive political issue for the latter.
Both leaders "expressed their condolences for the victims of the tragic events in the Channel yesterday and last week", they said, referring to the deaths of several migrants.
They committed "to strengthening their cooperation on irregular migration and the fight against criminal gangs responsible for this tragic loss of life through small boat crossings."
"If we want to fix the situation in the Channel, it's not just a bilateral situation," Macron told reporters.
"It's how to work much more efficiently with the European countries of first entry and with all the different countries in order to clearly fight efficiently against all the smugglers."
Starmer earlier said there was "no easy silver bullet" to stop small boats making the perilous crossing.
The two leaders met on the sidelines of the European Political Community (EPC) summit held near Oxford in England, their first meeting since Starmer's Labour government was elected two weeks ago.
They said they shared "the ambition to reinvigorate their defence cooperation" and their "steadfast support for Ukraine" as it fights off the Russian invasion.
The French president said it was "a very important moment, to have this reset" of Franco-British relations and of ties between the UK and the EU.
At the same time he called on the British to "respect what was decided and signed" during the laborious negotiations that followed their exit from the EU.
Starmer and Macron said they would hold a bilateral summit in 2025. The last Franco-British summit was in 2023 under the UK's then-prime minister Rishi Sunak.
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