The effect of surface functionalisation of bacterial cellulose nanofibrils (BC) and their use as reinforcement for polylactide (PLLA) nanocomposites was investigated. BC was functionalised with various organic acids via an esterification reaction. This rendered the otherwise hydrophilic BC hydrophobic and resulted in better compatibility (interfacial adhesion) between PLLA and BC. A direct wetting method, allowing the determination of the contact angle of polymer droplets on a single BC nanofibre, was developed to quantify the interfacial adhesion between PLLA and functionalised BC. It was found that the contact angle between PLLA droplets and functionalised BC decreased with increasing chain lengths of the organic acids used to hydrophobise BC. A novel method to compound BC with PLLA based on thermally induced phase separation (TIPS) to yield a dry form of pre-extrusion composite was also developed. The mechanical properties of the surface functionalised BC reinforced PLLA nanocomposites showed significant improvements when compared to neat PLLA and BC reinforced PLLA. The thermal degradation and viscoelastic behaviour of the nanocomposites were also improved over neat PLLA.