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Waldo was first settled in 1806, and was incorporated into a town and named Waldo on March 17, 1845.
The area was once part of the Waldo Patent, a large tract of land owned by Brigadier-General Samuel Waldo of Boston. It was first settled in 1811 by Henry Davidson, then organized as Waldo Plantation on July 6, 1821. The town was incorporated by the legislature on March 17, 1845, taking the name of its early proprietor.
A large portion of Waldo was rocky and uneven, unfit for cultivation. Some parts had arable soil, however, producing excellent farms and prosperous farmers. The town became noted for prize-winning cattle. It was also known for its forests, with much of the timber used for Belfast shipbuilding. The Wescott Stream provided water power, and by 1859 Waldo had seven busy sawmills. It also had one gristmill, some shingle machines, and a tannery. In 1870, the Belfast & Moosehead Lake Railroad began operating, its trains passing through the town.