AbstractThe covalent integration of inorganic nanoparticles in polymer matrices has gained significance for improving the structural properties of polymer-based materials. Here we report on the performance of poly(ω-pentadecalactone) networks with magnetite nanoparticles as netpoints in their magnetically-controlled shape-memory capability. Hybrid nanocomposites with magnetite nanoparticle content ranging from 5 to 11 wt% were prepared by reacting two types of oligo(ω-pentadecalactone) (OPDL) based precursors with terminal hydroxy groups, a three arm OPDL (3AOPDL, Mn = 6000 g mol−1) and an OPDL (Mn = 3300 g mol−1) coated magnetite nanoparticle (∅ = 10 nm), with a diisocyanate. Homogenous hybrid nanocomposites were obtained independent from the weight content of the OPDL decorated nanoparticles in the samples. At 100 °C (T > Tm-OPDL) the covalent integration of the nanoparticles increased the mechanical strength with increasing weight content whereby the elasticity remained almost constant. In magnetically-controlled one-way dual-shape experiments the shape fixity decreased from 95% to 90% but the shape recovery increased slightly from 95% to 97% when the nanoparticle content was increased. In magnetically-controlled reversible dual-shape experiments the nanoparticles had a restraining effect and the maximum shape-change of 65% for hybrid nanocomposites with 5 wt% magnetite nanoparticles was reduced to 36% when the particle content was increased to 11 wt%. These results show that the performance of hybrid nanocomposites can be tailored by nanoparticle content, however in terms of their applicability either mechanical strength or actuation capability should be focussed in the material selection.