The area has been inhabited since the Stone Age. In June 2008, a 6,000 year old spearhead was found at Marshall Street Park. The inhabitants of the area at the time of Spanish exploration were the Tocobaga Indians, who lived in villages around Tampa Bay. They were known for constructing various ceremonial and communal mounds, one of which is still visible in Safety Harbor's Phillippe Park. In 1528 Spanish explorer Panfilo de Narvaez landed in the area followed by Hernando De Soto in 1539. Safety Harbor(formerly known as Worth's Harbor) was first homesteaded by Count Odet Philippe, a Frenchman who is credited with introducing the grapefruit to Florida in 1823.

Safety Harbor is the home of the historic Espiritu Santo Springs, or "Springs of the Holy Spirit", a natural mineral spring. Its waters were given this name in 1539 by the Spanish explorer Hernando de Soto, who was supposedly searching for the mythical "Fountain of Youth". Prior to the Spanish exploration of Florida, the Tocobaga and Timuquan Indian tribes are believed to have fished and bathed in the spring's waters.

In the twentieth century, Espiritu Santo water was bottled and sold commercially and, later, a health spa and hotel were built over the springs. The Safety Harbor Resort and Spa, as it is now known, continues to be a prominent visitor attraction in Pinellas County.

In 1964, the site was designated a Historical Landmark by the U.S. Department of the Interior and, in 1997, a Florida Heritage Landmark.

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