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We aim to present 70 spectra of 68 new high-redshift type Ia supernovae(SNeIa) measured at ESO's VLT during the final two years of operation(2006-2008) of the Supernova Legacy Survey (SNLS). We use the full five yearSNLS VLT spectral set to investigate a possible spectral evolution of SNeIapopulations with redshift and study spectral properties as a function oflightcurve fit parameters and the mass of the host-galaxy.  Reduction and extraction are based on both IRAF standard tasks and our ownreduction pipeline. Redshifts are estimated from host-galaxy lines wheneverpossible or alternatively from supernova features. We used thespectrophotometric SNIa model SALT2 combined with a set of galaxy templatesthat model the host-galaxy contamination to assess the type Ia nature of thecandidates.  We identify 68 new SNeIa with redshift ranging from z=0.207 to z=0.98(<z>=0.62). Each spectrum is presented individually along with its best-fitSALT2 model. The five year dataset contains 209 spectra corresponding to 192SNeIa identified at the VLT. We also publish the redshifts of other candidates(host galaxies or other transients) whose spectra were obtained at the sametime as the spectra of live SNe Ia. Using the full VLT SNeIa sample, we buildcomposite spectra around maximum light with cuts in color, lightcurve shapeparameter ('stretch'), host-galaxy mass and redshift. We find that high-z SNeIaare bluer, brighter and have weaker intermediate mass element absorption linesthan their low-z counterparts at a level consistent with what is expected fromselection effects. We also find a flux excess in the range [3000-3400] A forSNeIa in low mass host-galaxies or with locally blue U-V colors, and suggestthat the UV flux (or local color) may be used in future cosmological studies asa third standardization parameter in addition to stretch and color.

The ESO's VLT Type Ia supernova spectral set of the final two years of SNLS