A novel mechanochemical (MC) method was examined for dechlorinating and recycling waste recording media tape. In this treatment, the tape was ground with CaO powder to decompose the constituent PVC. The ground sample was then washed with water to dissolve soluble chloride compounds formed during the MC treatment and filtered. The filtrated contained mainly calcium ions (Ca2+) besides the metals such as Co and Fe derived from the recording media, and thus it can be added to liquid containing phosphate ions (PO43-) to synthesize hydroxyapatite. The solid residue of filtration can be used for thermal recycling, because it does not contain any chlorine, and it has almost the same calorific value as RDF (refuse-derived fuel). Thus, the proposed MC method would be suitable for environmentally friendly treatment of waste recording media and their recycling.