We present evidence that the cosmological mean metallicity of neutral atomic hydrogen gas shows a sudden decrease at z > 4.7 down to Z = −2.03 +0.09 −0.11 , which is 6σ deviant from that predicted by a linear fit to the data at lower redshifts. This measurement is made possible by the chemical abundance measurements of eight new damped Lyα (DLA) systems at z > 4.7 observed with the Echellette Spectrograph and Imager on the Keck II Telescope, doubling the number of measurements at z > 4.7 to 16. Possible explanations for this sudden decrease in metallicity include a change in the physical processes that enrich the neutral gas within disks, or an increase of the covering factor of neutral gas outside disks due to a lower ultraviolet radiation field and higher density at high redshift. The later possibility would result in a new population of presumably lower metallicity DLAs, with an increased contribution to the DLA population at higher redshifts resulting in a reduced mean metallicity. Furthermore, we provide evidence of a possible decrease at z > 4.7 in the comoving metal mass density of DLAs, ρ metals (z) DLA , which is flat out to z ∼ 4.3. Such a decrease is expected, as otherwise most of the metals from star-forming galaxies would reside in DLAs by z ∼ 6. While the metallicity is decreasing at high redshift, the contribution of DLAs to the total metal budget of the universe increases with redshift, with DLAs at z ∼ 4.3 accounting for ∼20% as many metals as produced by Lyman break galaxies.