Male tiger Asim was brought to the zoo from a safari park in Denmark 10 days ago in attempts to be "the perfect mate" for long-term resident Melati.
After spending time apart in the tiger enclosure to get used to the new surroundings - the two were introduced to each other earlier.
But tensions "quickly escalated", became "more aggressive" and Melati died in a fight, the zoo said.
A statement issued by the zoo said Asim was immediately moved to a separate paddock and despite the best efforts of the vets, 10-year-old Melati died.
It added: "Our focus right now is on caring for Asim, as we get through this difficult event."
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The zoo's previous male, Jae Jae - which had fathered five cubs previously with Melati - was moved to French zoo Le Parc des Félins, on 30 January.
In 2013, Melati gave birth to two cubs - but one died after falling into a pool and drowning at the zoo.
Melati then gave birth to three more tiger cubs in February 2014.
The entire birth was monitored using hidden cameras.
The Sumatran tiger, which naturally lives in the forests and jungles of Sumatra, Indonesia, is now classified as critically endangered on the International Union for Conservation of Nature Red List of Threatened Animals.
According to London Zoo, the Sumatran tiger faces threats of poaching and habitat loss.
When in captivity, they can live for about 20 years.
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Sorry, media tags keep getting added to the url when I hit submit even if I type in the url instead of pasting it. Guess you'll have to message me if you want the link.
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