Spray drying of complex liquids to form solid powders is important in many industrial applications. One of the challenges associated with spray drying is controlling the morphologies of the powders produced; this requires an understanding of how drying mechanics depend on the ingredients and conditions. We demonstrate that the morphology of powders produced by spray drying colloidal polystyrene (PS) suspensions can be significantly altered by changing the molecular weight of dissolved poly(ethylene oxide) (PEO). Samples containing high-molecular-weight PEO produce powders with more crumpled morphologies than those containing low-molecular-weight PEO. Observations of drying droplets suspended by a thin film of vapor suggest that this occurs because the samples with high-molecular-weight PEO buckle earlier in the drying process when the droplets are larger. Earlier buckling times are likely caused by the decreased stability, demonstrated by bulk rheology experiments, of PS particles in the presence of high-molecular-weight PEO at elevated temperatures. We present a consistent picture in which decreased particle stability hastens droplet buckling and leads to more crumpled powder morphologies; this underscores the importance of interparticle forces in determining the buckling of particle-laden droplets.