Natural fibres, such as flax and hemp, are typically chosen as reinforcing elements in composites to replace traditional glass fibres due to their high stiffness, strength and low strain to failure. Some plant fibres such as coir and celery however possess high strains to failure, which could be utilised in a composite to enhance toughness. This paper reports on the use of Raman spectroscopy to follow the molecular deformation of single fibres of coir and celery. The technique is also used to characterise the orientation of the cellulose structure within the fibres. It is shown by mechanical testing of fibres that both celery and coir possess a non-linear stress-strain curve. Coir fibres however exhibit high strain to failure, whereas celery fibres are shown to have a much lower value of this parameter, despite having a similar coiled fibrillar structure. It is shown by using polarised Raman spectroscopy, and rotating the specimens with respect to the polarisation axis of the laser and measuring the intensity of the 1095 cm -1 Raman band, that both celery and coir fibres combine both axial and transverse orientation, due to their coiled structures. This is also confirmed by birefringence measurements. By following the shift in the central position of this Raman band as a function of cyclic deformation of the fibres, it is shown that the coir fibres recover their molecular deformation, whereas the celery does not show the same level of recovery. This difference between the fibres is postulated to be due to the fact that coir possesses an interlaced fibrillar structure, which remains intact, whereas the celery sub-fibrils unravel and orient towards the fibre axis during deformation.