The rheological, structural, and stress evolution of aqueous alumina (Al2O3):latex tape-cast layers of varying composition were studied by shear rheology, direct visualization, and a controlled environment stress measurement device. Their low shear viscosity was nearly independent of the alumina:latex ratio for binary mixtures whose particle size ratio (lambda = (D) over bar (alumina):($) over bar(D) over bar (latex)) approached unity, but varied over an order of magnitude for systems with particle size asymmetry. Direct visualization of these mixtures revealed that particle flocculation occurred as their total solids loading increased. Their structure was characterized at intermittent points during the drying process by imaging freeze-dried samples using scanning electron microscopy (SEM). Their corresponding stress histories exhibited three distinct regions: an initial period of stress rise, followed by a stress maximum, and, finally, a period of stress decay. Pure alumina layers exhibited a maximum stress of similar to1 MPa and a residual stress below 0.01 MPa. Pure latex films exhibited a maximum stress of similar to0.1 MPa and only a slight stress decay. The ceramic phase dominated the initial period of stress rise, while the latex phase strongly influenced the residual stress of composite layers cast from alumina:latex suspensions. Their maximum drying stress increased with decreasing Al2O3 particle size, whereas their residual stress increased with increasing latex T-g.