In this thesis, I study the self-assembly of monodisperse colloidal particles on liquid-liquid interfaces. Specifically, I examine the relevant parameters that govern the size of self-assembled clusters when they pass through a liquid-liquid interface. I first describe a millimeter length-scale self-assembly system, where I find that the number of particles within a sinking cluster is proportional to a power law of the dimensionless Bond number. I find that the sphere deposition geometry also plays an important role, where I observe distinctly different scaling for monolayer rafts in comparison to stacked sphere clusters. I then develop an analogous microfluidic self-assembly system, where I use a magnetic field gradient to self-assemble paramagnetic microparticles on an aqueous two-phase liquid-liquid interface. Here, I observe empirically that the number of particles within a microparticle cluster scales inversely with the
magnetic Bond number.