Additive friction stir deposition (AFSD), in which molten metal materials are formed into free-form stacked structural parts according to the path design, may have a wide range of applications in high-efficiency mass production. In this study, experiments were conducted for the rotational speed in the AFSD parameters of 6061 aluminium alloy bars to investigate the effects of different rotational shear conditions and heat inputs on the properties of the deposited layer for diameter bars based on the analysis of the micro-morphology, micro-tissue composition, and mechanical properties. The width and thickness of each layer were constant, approximately 40 mm wide and 2.5 mm thick. The particle undulations on the surface of the deposited layer were positively correlated with the AFSD rotational speed. Continuous dynamic recrystallisation in the AFSD process can achieve more than 90% grain refinement. When the rotational speed increases, it causes localised significant orientation and secondary deformation within the recrystallised grains. The ultimate tensile strength of the deposited layer was positively correlated with the rotational speed, reaching a maximum of 211 MPa, and the elongation was negatively correlated with the rotational speed, with a maximum material elongation of 37%. The cross-section hardness of the deposited layer was negatively correlated with the number of thermal cycles, with the lowest hardness being about 45% of the base material and the highest hardness being about 80% of the base material.