Although mechanical pulp can be considered as a potential raw material for preparation of microfibrils, suitable pre-treatment methods have been missing. Consequently, the objectives of this study were firstly to find a suitable procedure to prepare lignocellulose microfibrils (LCMF) from fractionated thermo-mechanical pulp (TMP) and secondly to evaluate if these TMP-based materials could be used as paper additives to increase paper strength. Carboxymethylation was found to be a suitable pretreatment for both TMP fines and TMP fibres to enable preparation of individualised LCMF after subsequent homogenisation treatment. After air drying, this material formed dense continuous films in conformity with films prepared from cellulose microfibrils (CMF) originating from chemical pulp. Homogenisation only or sulphonation followed by homogenisation did not fibrillate the TMP samples into individualised LCMF. Analysis of paper properties showed that addition of 20% LCMF to a standard TMP furnish improved tensile strength index by 15%. The LCMF-containing papers were also more brittle (less elongation) than the other paper sheets in this study. Similar tensile strength index was also obtained for TMP fines treated by sulphonation followed by homogenisation.