Nearly 1,700 of the record 11,000 applications received by Surrey County Council came from bordering London boroughs like Croydon, Sutton and Kingston-upon-Thames.
They account for 15% of the total submitted by the closing date for places in the next academic year.
A large number of the applications were for schools in Caterham, Epsom, Esher and Sunbury-on-Thames.
Around 1,000 forms were submitted by Surrey parents to schools in London boroughs.
A similar number of applications were received from London boroughs last year.
The news comes after estate agents predicted a trend that has seen Londoners leave the capital for Surrey will continue.
More than 90% of Surrey secondaries are rated outstanding or good, according to Ofsted.
Surrey County Council Council’s Cabinet Member for Schools and Learning Linda Kemeny said: “Surrey has some of the best state schools in the country and it’s clear that the high quality education they offer continues to attract a large number of Londoners.
“Surrey needs to find 13,000 extra places in the coming years and unprecedented demand has left the council with a £215 million funding shortfall.
“With the county’s taxpayers contributing £6 billion to the national coffers every year and getting less than a billion back in funding for services, it’s time Whitehall gave Surrey’s schools a fairer deal.”