We report controlled syntheses of super-aligned carbon nanotube (CNT) arrays with the desired tube-diameter, number of walls, and length for spinning continuous unidirectional sheets to meet a variety of industrial demands. The tube-diameter distribution of super-aligned arrays is well controlled by varying the thicknesses of catalyst films, and the length of them is tuned by the growth time. Further investigation indicates that the physical properties of the unidirectional sheets, such as electrical transport, optical transmittance, and light emission properties, can be well tuned by the tube-diameter- and length-controlled growth. This work extends the understanding of the super-aligned CNT arrays and will be very helpful in developing further applications.