The Călimani National Park (CNP), legally founded in 2000 in order to ensure the highest level of protection for the unique natural and scientific values it hosts, is the largest protected volcanic area in Romania. It covers a significant part of the Călimani Mountains representing the largest, highest, and most voluminous segment of the Neogene Călimani-Gurghiu-Harghita volcanic range. The natural values under protection in the CNP include the unique high-mountain volcanic landscape hosting glacial and periglacial features, lakes and marshes, spectacular rock formations, and unique floral elements. Due to their outstanding scientific value, the botanical Science Reserve of Juniperus with Pinus cembra, the geographical Iezer Lake Science Reserve, and the geological “12 Apostles” Science Reserve are subject to the highest legal level of protection. CPN also hosts damaged natural values of geoheritage importance. This is the place where the phenomenon of volcanic karst was described for the first time, and the term “vulcanokarst” coined. Open-pit sulfur mining destroyed its original features and only poor traces of them can be found today. The high-mountain volcanic landscape was also catastrophically damaged by mining. However, remediation and re-cultivation activities in the open-pit area significantly attenuated the damage. Little attention is paid by the Park’s management to the valuation of the geological and volcanological features deserving higher levels of protection. Most of them are not even known to the wider public, with the exception of geologists. Touristic valuation of the area was recently enhanced by the remediation of the old “Maria Theresia road” linking Transylvania and Bukovina across the mountains. There is still a lot to do in order to fully take advantage of the natural values of geoheritage relevance hosted by the CNP, in teaching, research and touristic/leisure activities. Actions to be undertaken to this end suggested here include organization of thematic workshops, conferences, exhibitions, and field practice for students, professionals and the general public focused on geoheritage values, placing geoeducational boards along touristic trails, devising field guides and promotional material, and connecting the Călimani Mts. to broader touristic networks such as the proposed “Pannonian volcano route.”