Among several ions playing a vital role in the body, Sr2+ and Mg2+ are involved in the mechanism of bone formation, making them especially useful for bone tissue engineering applications. Recently, polylactic acid (PLA)/Mg composites have emerged as a promising family of biomaterials due to their inherent biocompatibility and biodegradability properties. In these composites, polymer and bio-metal have a synergetic effect—while the PLA inhibits the Mg fast reactivity, Mg provides bioactivity to the inert polymer buffering the medium pH during degradation. Meanwhile, the typical form of administrating Sr2+ to patients is through the medication strontium ranelate (SrR), which increases the bone mineral density. Following this interesting research line, a new group of composites, which integrates Mg particles and SrR charged onto halloysite nanotubes (HNT) in a polymeric matrix, was proposed. PLA/Mg/SrR–HNT composites have been processed following a colloidal route, obtaining homogenous composites granulated and film-shaped. The drug delivery profile was evaluated in terms of in vitro lixiviation/dissolution paying special attention to the synergism of both ions release. The combination of two of the most reported ions involved in bone regeneration in the composite biomaterial may generate extra interest in bone healing applications.