He was forced to ditch into the sea. He was later rescued by a chopper, reports The Mail.
Rossy — known as Jetman — was aiming to cross from Africa to Europe with just the wing strapped to his back.
But about 15 minutes after he took off from above Tangier in Morocco, organisers wrote on the micro-blogging website Twitter: "He may be in the sea. We have search and rescue team in place."
TV and internet viewers saw Rossy alive in the sea after his landing.
Last year he amazed the world when he flew from Calais to Dover crossing the English Channel.
The 50-year-old jumped from a plane at 6,500ft to start today's record bid.
He was intending to use his four-cylinder jet pack to power the eight-foot carbon fibre wing at speeds of up to 180mph across the 23 miles from outside Tangier to Atlantera in southern Spain.
But he never made it across and ditched in the sea.
Organisers said Rossy had deployed his parachute and it appeared that both he and the wing "seemed intact".
A search and rescue team codenamed Falcon 1, involving former special forces members, later winched him to safety.
Before setting off the Swiss airline pilot and aviation inventor said: "It's going to be historic" before adding "no-one has ever done this before".
Rossy had hoped to land safely on a beach in Spain after flying for about 15 minutes.
The wing — which was designed by Rossy — weighs around 60kg but because of the dangers involved he wears a flame retardant suit.
Rossy was followed throughout the attempt by a team of paramedics in a helicopter.
In September last year, Rossy cracked open the Champagne as he became the first person to fly solo across the English Channel using the single jet-propelled wing.
A global audience witnessed Rossy leap from a plane more than 8,200ft (2,500m) above France before soaring at more than 100mph over one of the world's busiest shipping lanes powered by four jets on his home-made wing.
Rossy, a former military pilot, traced the route of French aviation pioneer Louis Bleriot, who became the first person to fly across the Channel in a plane 99 years earlier.
On Wednseday, efore making his record-breaking attempt, he told Sky News: "You don't have this chance many times in your life, so you take it when it's here."