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Cambridge Springs in Crawford County was settled early in the 1800s by German and Irish families, most of whom purchased their sites through the Holland Land Company. The land was fertile for growing grains. French Creek, which flowed through from the northeast, was an ample source of water. The first bridge over the creek was built in 1815.

Growth was slow and due to disputes over land claims, some of the early settlers were dispossessed. However, because the small community lay along the route between Meadville and Waterford, it benefited by the stagecoach service between those areas.

In 1853 Cambridge Township was organized from a part of Venango Township to the west. Nine years later the Atlantic & Great Western Railroad (A&GWRR) laid tracks northward to communities in eastern Erie County and beyond. After the drilling of the first successful oil well near Titusville to the east, the east-west Pennsylvania Petroleum Railroad tracks were laid and the two sets of tracks crossed in the midst of the growing village. In 1866 the village incorporated as Cambridgeboro.

With the interest in oil, local resident, Dr. Gray, sunk a well in 1860, only to hit a mineral spring. Not until a national zeal for mineral waters became popular did Gray attempt to market his. In 1884 he opened his first springhouse and two years later the Riverside Hotel, one of earliest of 40 hotels and boarding houses in the borough was built. By this time businesses in the community also included warehouses, many and various mills, blacksmith shops, shoe shops, a tannery, a marble works, clothing and drug stores, dry goods and hardware store, groceries, millineries, bakeries, a meat market, the first cheese factory in Crawford County, and more.

The A&GWRR became the New York, Pennsylvania & Ohio Railroad (NYP&ORR) by 1895 and was bringing in visitors to the springs at a rate of one trainload per hour during the season. A sign was soon erected along the tracks near the depot notifying travelers that at this point they were halfway between New York and Chicago.

During the craze, mineral waters were regarded as valuable in the cure of rheumatism, gout, constipation, indigestion, malaria, nervous prostration, bilious derangement, catarrhal conditions of the bladder and kidney, diabetes and Bright's Disease. To acknowledge the importance of the springs to the community, the name was changed in 1897 to Cambridge Springs. At least a dozen springs were in operation in and around the community by this time.