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Shere Khan is depicted by Kipling as having been born with a crippled leg, so his mother gave him the derisive nickname "Lungri" ("The Lame One"). Despite this condition, Shere Khan is prideful and regards himself as the "rightful" lord of the jungle. The only creature who looks up to him is Tabaqui, a spineless and hated golden jackal.

In "Mowgli's Brothers", Shere Khan's failed attempt to hunt humans causes a human "cub" to stray from its parents. When Shere Khan discovers the infant, it has been adopted by Indian wolves, Raksha and Father Wolf, who have named the child Mowgli. Mowgli is accepted into Akela's wolf pack and is protected by Bagheera (a panther) and Baloo (a bear). Furious at losing his kill, the tiger swears that the boy will be his some day. While Mowgli is growing up, Shere Khan infiltrates the wolf pack by promising the younger wolves rich rewards once Akela is deposed. When the young wolves manoeuvre Akela into missing his kill, the pack council meets to kill and replace him. Shere Khan threatens to take over their hunting territory if the wolves do not give him Mowgli. Having been warned by Bagheera, Mowgli attacks Shere Khan and his allies with a burning branch (the mysterious and powerful "red flower" of man) and drives them away. Akela leaves the pack to become a lone hunter. Mowgli goes to the human village but swears that he will return one day with Shere Khan's skin and lay it upon Council Rock.

Shere Khan also appears in the story "How Fear Came", which is set between the first and second halves of the "Mowgli's Brothers", and probably sometime after "Kaa's Hunting". In this story, the tiger comes to drink from the river just after having killed a human purely for sport, leading Hathi the elephant to tell the story of why tigers, out of all the animals in the jungle, are allowed to hunt humans for pleasure at certain times. This story, in which Mowgli appears mainly as an observer, may be seen as a direct ancestor of Kipling's Just So Stories.

In "Tiger! Tiger!", Mowgli is adopted by Messua and her husband and learns human ways. In this short story, Mowgli learns that the villagers have heard of the tiger Shere Khan, who also has a bounty on his head, but believe that the tiger is lame because he is the reincarnation of a money-lender injured in a riot. When Mowgli scoffs at these fanciful tales, the villagers decide to put him to work herding buffalo. He then meets his wolf friend Grey Brother, who tells him that Shere Khan is still planning to kill him. Grey Brother forces Tabaqui to tell him where and when Shere Khan is planning to strike, then kills the jackal. With the help of Akela, Grey Brother and Mowgli trap Shere Khan in a narrow canyon and incite the buffalo to stampede him to death. Mowgli then skins Shere Khan's hide, briefly interrupted by the arrival of the village hunter Buldeo, who tries to take the tiger's skin for himself only to be driven off by Akela. At the end of the story, Mowgli makes good on his promise and lays the skin of Shere Khan upon the Council Rock and dances upon it in victory before the wolves.