Shamir, who had Alzheimer's disease, died Saturday at a nursing home in the town of Herzliya, north of Tel Aviv. His death was announced by the Israeli government.
In a statement, Israeli Prime Minister Benjamin Netanyahu called Shamir one of the "giants" who "established the state of Israel and fought for the freedom of the Jewish people in its land."
Shamir, who emigrated from Poland 13 years before Israel's independence, belonged to the generation of Israelis who went on to lead the nation they had helped to create. But unlike some others from that era, the diminutive Shamir held fast to his hard-line views after climbing the Israeli political ladder to become prime minister for four terms during the 1980s and early 1990s.
His pugnacious attitude toward Arabs often put him at odds with U.S. officials, who saw him as an impediment to reconciliation with the Palestinians.
Shamir only grudgingly took part in a pivotal 1991 peace conference in Madrid that opened the way for talks with the Palestinians and led to a peace treaty with Jordan.
His tough-nosed views made him a darling of Jewish settlers and kept him atop the right-wing Likud Party for a decade after Menachem Begin, the former prime minister, stepped aside in 1983.
To the end of his life, Shamir never wavered in his defense of Jewish settlement in the West Bank and Gaza Strip even though other hawkish Israeli leaders, such as Ariel Sharon, came to conclude that Israel was better off letting go of some areas. Shamir, whose parents and sisters died during the Holocaust, saw all the land between the Jordan River and the Mediterranean Sea as a Jewish birthright.
"The settlement of the Land of Israel is the essence of Zionism," Shamir said in 1997, after his retirement from public life. "Without settlement, we will not fulfill Zionism. It's that simple."
Born Itzhak Yezernitksy on Oct. 15, 1915, in present-day Belarus, Shamir was a 20-year-old university student when he arrived in what was then British-governed Palestine. Working variously as a construction worker and clerk, Shamir joined an underground movement of a hard-line school of Zionists known by its Hebrew acronym, Etzel.
When the group split in 1940, Shamir went with the more militant Lehi branch, which battled Arabs and launched attacks against the British military. The group, also known as the Stern Gang, drew inspiration from the Irish Republican Army. Shamir's nom de guerre was "Michael," after Irish revolutionary leader Michael Collins.
Shamir was a leader of the band at a time when its operations included the 1944 assassination of Lord Moyne, the British minister in Palestine, and the 1948 killing of Count Folke Bernadotte, a Swedish nobleman who served as the United Nations' representative in the region. Shamir's role was never definitively established.
Shamir was arrested twice by the British but escaped both times. Lehi disbanded after Israel achieved statehood.
During the 1950s, Shamir joined the Mossad spy agency, heading a team in Europe. He later moved into politics, joining the Herut Party under Begin. He won a seat in the Israeli parliament in 1973 as a member of Likud, which had merged Herut and smaller rightist groups.
Likud upended Israeli politics in 1977 when it defeated the long-dominant Labor Party, thrusting Begin into the prime minister's slot. Shamir became speaker of the parliament, or Knesset. Six years later, he inherited Likud, and the prime minister's job, when Begin abruptly quit a year after the invasion of Lebanon.
But a slew of economic troubles, including triple-digit inflation, took a toll on Shamir's standing, and he was forced to spend the rest of the decade in a coalition with the left-leaning Labor in order to keep power. He and Peres agreed to share the post for a term by taking turns as premier for two years each beginning in 1984.
Shamir opposed rapprochement with Israel's Arab neighbors and responded forcefully when the first Palestinian intifada erupted in 1987. Addressing settlers from atop a West Bank castle at the time, he vowed that "anybody who wants to damage this fortress and other fortresses we are establishing will have his head smashed against the boulders and walls."
His backing for the settlements and refusal to negotiate with the Palestinians put him at odds with the administration of President George H.W. Bush, which was promoting a peace process after the Palestine Liberation Organization recognized Israel's right to exist in 1988.