Jumbo squid mantle muscle gels were prepared by using the one-step (90 °C/30 min) and the two-step (30 °C/1 h + 90 °C/30 min) heat treatments (HTs) with and without the addition of D-isoascorbic acid (IAA). Reactive sulfhydryl (-RSH) content, SDS-PAGE protein profiles, gel-forming ability in terms of their texture profile analysis (TPA), folding test (FT), and water holding capacity (WHC) were evaluated on experimental gels. Additionally, the rheological and calorimetric behaviors of previously prepared sols were monitored. The −RSH content of gels showed no statistical differences (p ≥ 0.05) due to the effect of HT; however, their content was reduced by 18.4% by the addition of IAA. The TPA showed changes only in cohesiveness (p < 0.05). The FT evaluation indicated that all gels were A−B grade. The WHC of gels increased with the two steps of HT but decreased with the addition of IAA. The rheology and calorimetry of sols remained without major variations.