Edmund, the British number three, went down 6-2 7-5 6-4 to France's Adrian Mannarino, the world number 55.
Defeat means the 21-year-old is still waiting for his first win in the men's singles at Wimbledon.
The Yorkshireman had the honour of being the first home player to walk out on to court, but was unable to provide a winning start for a partisan crowd on court two.
Ranked 13 places below his opponent, he lost his serve early in the first set and never recovered in an edgy display.
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