The 2000 George Bush vs. Al Gore election, also, the 1888 (Rebulican Benjamin Harrison vs Democrat Grover Cleveland) and 1876 (Rebulican Rutherford B. Hayes vs. Democrat Samuel J. Tilden) elections.
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The winner of the popular vote lost the election. The most unusual aspect was the involvement of the Florida Supreme Court and the US Supreme Court in the adjudication of irregular votes that could have changed the result of the election.
No US president was elected unanimously by popular vote. The only president elected unanimously by the electoral college was George Washington (There was no popular vote in this election).
21 or older
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the electoral college is most likely the most unique. As it is possible to lose the popular vote for President but still win the election by the electoral college.