Tightly focusing a continuous-wave, near-infrared laser beam at the air/solution interface of a millimeter-thick layer of glycine in D2O forms a crystal through a polymorphically and spatially controlled nucleation process known as gradient-force laser-induced nucleation or optical-tweezer laser-induced nucleation. However, when this same beam is focused at the glass/solution interface of a film of aqueous glycine, a highly concentrated laser-induced phase-separated (LIPS) solution droplet is formed that does not nucleate while the focusing beam remains on. Two competing theories have emerged about the nature of the LIPS droplet: one proposes that it is a merger of prenucleation metastable nanodroplets and clusters into one large homogeneous “dense liquid droplet”, and the other stipulates that it is the result of the partitioning of larger droplets into the new phase, but not a merging of droplets, around the focal point of the beam. In order to determine the nature of the LIPS droplet, dynamic light scattering was used to detect the presence of nanodroplets undergoing Brownian motion within the droplet and to measure their relative size following a range of laser exposure times. The observation of nanodroplets in motion in the center of the LIPS droplet revealed that the application of optical tweezers at the glass/solution interface forms a relatively monodisperse collection of large nanodroplets (>700 nm) concentrated around the focal point of the beam with smaller particles (<100 nm) depleted within the first 2 min of laser exposure. The LIPS droplet quickly reaches a steady state and is not affected by increasing focusing times. These findings allow for a better understanding of the interactions of optical tweezers with aqueous glycine nanodroplets. This understanding will help in studying the fundamental nature of metastable nanodroplets. More practically, laser-induced phase separation makes possible the nucleation-free separation of large nanodroplets from small clusters, facilitating materials technologies such as high purity, polymorphically selective nucleation of crystals and co-crystals used for pharmaceuticals, dyes, and photovoltaics.