This work evaluated for the first time the effect of dual modification of cassava starch by using ozone (O-3) and dry heating treatment (DHT). The dual modification was capable to promote fissures on the surface of the starch granule (DHT + O-3), affected the starch amorphous domains, presented greater degree of starch oxidation (DHT + O-3) and different profiles of starch molecular size distribution. These modifications resulted in starches with different properties. Moreover, the sequence of treatments was decisive for the hydrogel properties: while DHT + O-3 resulted in formation of stronger gels, O-3 + DHT resulted in weaker gels. In conclusion, this proposed dual modification was capable to produce specific modified starch when compared with the isolated treatments, also expanding the potential of cassava starch applications.