Green energy-storage materials enable
the sustainable use of renewable
energy and waste heat. As such, a form-stable phase-change nanohybrid
(PCN) is demonstrated to solve the fluidity and leakage issues typical
of phase-change materials (PCMs). Here, we introduce the advantage
of solid-to-gel transition to overcome the drawbacks of typical solid-to-liquid
counterparts in applications related to thermal energy storage and
regulation. Polyethylene glycol (PEG) is form-stabilized with cellulose
nanofibrils (CNFs) through surface interactions. The cellulosic nanofibrillar
matrix is shown to act as an organogelator of highly loaded PEG melt
(85 wt %) while ensuring the absence of leakage. CNFs also preserve
the physical structure of the PCM and facilitate handling above its
fusion temperature. The porous CNF scaffold, its crystalline structure,
and the ability to hold PEG in the PCN are characterized by optical
and scanning electron imaging, infrared spectroscopy, and X-ray diffraction.
By the selection of the PEG molecular mass, the lightweight PCN provides
a tailorable fusion temperature in the range between 18 and 65 °C
for a latent heat storage of up to 146 J/g. The proposed PCN shows
remarkable repeatability in latent heat storage after 100 heating/cooling
cycles as assessed by differential scanning calorimetry. The thermal
regulation and light-to-heat conversion of the PCN are confirmed via
infrared thermal imaging under simulated sunlight and in a thermal
chamber, outperforming those of a reference, commercial insulation
material. Our PCN is easily processed as a structurally stable design,
including three-dimensional, two-dimensional (films), and one-dimensional
(filaments) materials; they are, respectively, synthesized by direct
ink writing, casting/molding, and wet spinning. We demonstrate the
prospects of the lightweight, green nanohybrid for smart-energy buildings
and waste heat-generating electronics for thermal energy storage and
management.