Carbon nanotube (CNT)/ composites were synthesized to enhance the hydrogen storage properties. The emphasis was made on the effect of different shortening methods of CNTs on the open-tip structure and the resulting properties. The use of open CNTs as a starting material resulted in an enhanced hydrogen properties of CNT/ composites. Among the employed methods for the shortening of CNTs, wet milling using ethanol was the most efficient, while ultrasonic acid treatment or thermal decomposition resulted in a less hydrogen storage capacity.