The potential of neutral sulphite pulps from softwood with different yields (c. 58–84%) and high residual lignin contents (c. 10–25 wt%) was investigated as a raw material for lignin-containing cellulose nanofibrils (LCNFs) by following their fibrillation during grinding. It was found that the lower yield (58–65%) pulps needed two grinding cycles to produce fibrillated fibers with water retention values (WRV) as high as 400 g/g (at the energy consumption level of 1400 kWh/t). In contrast, the high yield (77–84%) pulps fibrillated more slowly, requiring five grinding cycles to reach comparable WRV values. Apparently, higher crosslinking degrees of lignin in the high yield pulps are hampering the fibrillation, although the high hemicellulose contents (21–24 wt%) and the high charge densities (200–350 µmol/g, originating from carboxylic and sulphonic acid groups) of the pulps were expected to enhance the fibrillation. Nevertheless, regardless of the different fibrillation behaviour, most of the pulps formed c. 10–15% of nanosized material below 30 nm and significant amounts of fibrils with size under 100 nm based on the centrifugation method and FE-SEM images. As the pulps were of moderate to high yield and fibrillated easily without any chemical or enzymatic pretreatments, they show promise for cost-efficient production of LCNFs. The nanopapers prepared from the fibrillated pulps showed tensile strengths (73–125 MPa) comparable with the nanopapers from high yield mechanical pulps, whereas the water contact angles (41°–58°) were closer the those of chemical pulps.