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Van Buren was initially the leading candidate for the Democratic party's nomination again in 1844, but his continued opposition to the annexation of Texas angered Southern Democrats, leading to the nomination of James K. Polk. Van Buren led a third-party ticket in 1848, and his candidacy most likely helped Whig nominee Zachary Taylor defeat Democrat Lewis Cass. Van Buren returned to the Democrats after 1848, but grew increasingly opposed to slavery, and became one of the party's outspoken abolitionists. He supported Abraham Lincoln's policies during the American Civil War. He died in Kinderhook in July 1862, at age 79.

However, his presidency soon eroded with his response to the Panic of 1837, which centered on his Independent Treasury system, a plan under which the Federal government of the United States would store its funds in vaults rather than in banks; more conservative Democrats and Whigs in Congress ultimately delayed his plan from being implemented until 1840. His presidency was further marred by the costly Second Seminole War (a result of continuing Jackson's Indian removal policy); and his refusal to admit Texas to the Union as a slave state, done as an attempt to avoid heightened sectional tensions. In 1840, a surge of new voters—who nicknamed him "Martin Van Ruin"—helped turn him out of office.

In his cabinet position, Van Buren became a key Jackson advisor, and built the organizational structure for the coalescing Democratic Party. He ultimately resigned to help resolve the Petticoat affair, and briefly served as the U.S. ambassador to the United Kingdom. At Jackson's behest, the 1832 Democratic National Convention nominated Van Buren for Vice President of the United States, and he took office after the Democratic ticket won the 1832 presidential election. With Jackson's strong support, Van Buren won the presidential nomination at the 1835 Democratic National Convention, and he defeated several Whig opponents in the 1836 presidential election.

As the leader of the Bucktails faction, Van Buren emerged as the most influential politician from New York in the 1820s and established a political machine known as the Albany Regency. Following the 1824 presidential election, Van Buren led to re-establish a two-party system with partisan differences based on ideology rather than personalities or sectional differences; he supported Jackson's candidacy in the 1828 presidential election with this goal in mind. He ran successfully for Governor of New York in order to support Jackson's campaign, but resigned shortly after Jackson was inaugurated so he could accept appointment as Jackson's Secretary of State.