This paper addresses the characterisation of the mode I interlaminar fracture toughness of a carbon fibre/epoxy composite material, toughened with thermoplastic particles in the ply interlayers. The characterisation is undertaken at −55 °C, 19 °C, and 90 °C, on both dry and fully moisture saturated coupons. Fractographic observations of the delamination surfaces allows identification of the failure mechanisms. The mode I propagation fracture toughness tested at wet/90 °C exhibits a 176% increase compared to the dry/19 °C specimens, due to enhanced plastic deformation of the interlayers and more prominent fibre bridging. Moisture-saturated coupons tested at −55 °C suffered a 57% reduction of mode I fracture toughness compared to those under dry/19 °C conditions. This is due to the dis-bond and consequent plucking of the thermoplastic particles from the surrounding matrix. This observation points to the fact that wet/cold conditions may represent the worst-case scenario for the interlaminar fracture performance of composite systems toughened with thermoplastic interleaves.