In this study, we report on the fabrication of photo/thermo dual stimulus-responsive liquid marbles (LMs) that can be disrupted by light irradiation and/or heating. To stabilize the LMs, we synthesized micrometer-sized stearic acid (SA) particles coated with overlayers of polypyrrole (PPy) by aqueous chemical oxidative seeded dispersion polymerization. The SA/PPy core–shell particles could adsorb at the air–water interface to stabilize LMs by rolling water droplets on the particle powder bed. The presence of SA, known as a phase-change material, which undergoes a transition from solid to liquid by heating, and PPy, which can transduce light to heat, gives rise to the photo and thermo dual stimulus-responsive characters of the LMs. The disruption of the LMs could be induced in a cascade manner: light irradiation on the LM induced a temperature increase, followed by melting of the SA component on the LM surface, leading to its disruption and release of the inner water. The disruption time is linked to the PPy loading and light irradiation power, and it can be tuned from quasi-instantaneous to a few tens of seconds. The melting of SA due to a light-induced phase change from the solid to liquid state is a new mechanism to trigger the disruption of LMs. We finally demonstrated two applications of the LMs as a light-responsive microreactor and a sensor.