Unleashing the potential of self-similar materials could prove as serious contenders for next-generation sensors. Herein, a systematic approach to design and develop self-similar nonwoven interfacially aided with multi-walled carbon nanotubes (SS–NI-MWCNTs) via a facile, scalable, and cost-effective vacuum filtration process has been proposed. A simple deformation mechanism of SS-NI-MWCNTs giving rise to the piezoresistive behaviour has been correlated with the tensile mechanics universal to both nonwovens and random arrays of MWCNTs. The failure of the SS-NI-MWCNTs is preponderantly governed through inter-tube/fibre sliding that originates from self-similar serpentine characteristics of random arrays of CNTs and glass fibre-based nonwoven materials, triggering their piezoresistive nature. The merits and limits of the sensing ability of esoteric SS-NI-MWCNTs have been demystified by artificially inducing various types of defects in the form of notches. The measured gauge factors of pristine and notched SS-NI-MWCNTs are found to be in the range of 18–30 at a 1% strain level.