The attachment of CMC to pulp is known to have a strong impact on the tensile strength properties. The mechanisms behind the strength-enhancing ability of the CMC have been investigated by studying the effect of surface carboxymethylation on some basic fibre and sheet properties. Standard methods were used for the strength evaluation, and the relative bonded area was determined from both light-scattering measurements and BET-analysis. The effect of CMC on the shear bond strength was calculated using Page’s equation. The attachment of CMC was shown to increase the shape factor and reduce the number of kinks per fibre, which is beneficial for the tensile strength. Surface carboxymethylation also increased the relative bonded area, but on a small-scale structural level detectable only using BET-analysis and not by the scattering coefficient. The sheet density was not affected by the treatment. CMC attachment also increased the shear bond strength. In order to use Page’s equation for this evaluation, the relative bonded area had to be determined by BET-analysis. The positive effect of CMC on sheet formation also contributed to an increase in tensile strength.