Energy efficient production of nanocellulose fibres is key to establishing this highly-promoted materials in an industrial scale. In this work, we attempt to explain how the mechanical energy input and the chemical composition of the raw materials affect the quality of nanofibres. Bleached eucalyptus Kraft (BEK) pulp, a commercially availble microfibrillated nanocellulose from cotton, and whitewater fines collected from a radiata pine thermomechanical pulping (TMP) mill were used to produce cellulose nanofibres. BEK was the most responsive to mechanical fibrillation due to low crystallinity and it produced high aspect ratio nanofibres, while TMP whitewater fines were the most difficult to process and resulted in low aspect ratio nanofibres. Nanofibres were then added to TMP newsprint to evaluate the effect on tnesile strength. Nanofibres produced from BEK were able to increase the tensile strength the most, while nanofibres from TMP whitewater fines had the least effect. The results showed that a high aspect ratio and a surface chemical composition favouring more hydrogen bonds i.e. pure cellulose, are the key criteria when selecting nanofibre for strength improvement in paper.