Spark plasma sintering (SPS) was used to fabricate Al/diamond composites. The influence of diamond particle size on the microstrueture and thermal conductivity (TC) of composites was investigated by combining experimental results with model prediction. The results show that both composites with 40 μm particles and 70 μm particles exhibit high density and good TC, and the composite with 70 μm particles indi-cates an excellent TC of 325 W·m~(-1)·K~(-1). Their TCs lay between the theoretical estimated bounds. In contrast, the composite with 100 μm particles demonstrates low density as well as poor TC due to its high porosity and weak interfacial bonding. Its TC is even considerably less than the lower bound of the predicted value. Using larger diamond particles can further enhance thermal conductive performance only based on the premise that highly dense composites of strong interfacial bonding can be obtained.