The giant Galapagos tortoises, which can live up to 200 years, were among the species that helped Charles Darwin formulate his theory of evolution in the 19th century.
The park is considering embalming George's body so that it can be displayed there.
A spokesman said the park plans to carry out a postmortem to determine what may have killed the tortoise.
Scientists had been trying to get George to mate since 1993. He was notoriously disinterested in the opposite sex and failed to produce any offspring.
The pen where George lived was visited by thousands of tourists every year, who often had to scramble over each other to take pictures of one of the rarest creatures on Earth.
The islands often attract celebrities, including Angelina Jolie and Brad Pitt, who visited earlier this year.
Sailors and fishermen hunted tortoises for their meat, to the point of extinction.
Their habitat has been eaten away by goats introduced from the mainland.
The Galapagos' giant tortoise population was decimated after the arrival of humans, but a recovery program run by the park and the Charles Darwin Foundation has increased the overall population from 3,000 in 1974 to 20,000 today.
The archipelago has been a UNESCO World Heritage Site since 1978 for the rich plant and animal life found both on its land and in the surrounding sea.
In 2007, the organization declared the island chain's environment endangered due to the increase of tourism and the introduction of invasive species.
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