Nowadays, it is greatly concerning the harmful effects provoked over the environment and citizens by the urban pollution of NOx (NO + NO₂) gases. With the aim to remediate this problem, photocatalytic Layered Double Hydroxides (LDH) have been applied recently to remove these pollutants (De-NOx action) directly from the air. In this work, Ni²⁺Ti⁺⁴ -LDH with the interlayer anion carbonate have been synthesized by the coprecipitation method (NiTi-LDH). In addition to this preparation procedure, a treatment, AMOST (Aqueous Miscible Organic Solvent Treatment) has been applied to the samples in order to increase its surface area and particle dispersion (NiTi-AM samples). Moreover, two Ni/Ti ratios have been prepared to examine its effect on the De-NOx performance. The samples were characterized in order to study its structure, porosity, morphology, and optical properties. The obtained results showed that the NiTi-AM chemical structure did not change after the AMOST, but they showed a high increase of the delamination degree, leading to high specific surface area values. The photocatalytic De-NOx performance increases in those samples with higher amount of Ti (Ni/Ti = 2/1) and those subjected to the AMOST process. This process had more effect on the Ni/Ti = 3/1 ratio samples exhibiting improved photoactivity (≈ 10 %) compared to those samples prepared by conventional method. The enhanced De-NOx performance was associated to the higher number of LDH nanosheets, which increases the number of actives sites accessible to the reactant molecules.