We used pendant droplet methods to measure the interfacial tension between aqueous colloidal solutions and 1-octanol and the surface tension of aqueous colloidal solutions. The filling volume fraction of colloids is 0.03, which was the same as that used for supraball assembly. Here, we used 219-nm SPs and 217-nm SMPs. For the surface tension measurements, we opened the droplet in a quartz cuvette to reduce evaporation. In the interfacial tension measurements, we made a saturated 1-octanol solution with an excess amount of water and then opened the aqueous droplet (with or without particles) in the saturated 1-octanol solution, so that there is little water diffusion into 1-octanol. We recorded the interfacial tension values and the droplet volume over a period of time (600 or 1400 s). The volume of droplets did not change, and thus the diffusion of water into 1-octanol (or vice versa) was negligible during the time scale of our measurements (fig. S6). As a control, we also measured interfacial tension between water and 1-octanol without any colloids.

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