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Due to global environmental concerns related to climate change, the need to improve the service life of structures and infrastructures is imminently urgent. Structural elements typically suffer service life reductions, leading to poor environmental sustainability and high maintenance costs. Graphene oxide nanosheets (GONSs) effectively dispersed in a cement matrix can promote hydration, refine the microstructure and improve interfacial bonding, leading to enhanced building materials’ performance, including mechanical strength and transport properties. Cement-based nanocomposites engineered with GONSs were obtained using two commercial nanofillers, a GO water suspension and a free-flowing GO nanopowder, characterized by fully comparable morphology, size and aspect ratio and different oxidation degrees (i.e., oxygen-to-carbon molar ratio), 0.55 and 0.45, respectively. The dosage of the 2D-nanofiller ranged between 0.01% and 0.2% by weight of cement. The electrical and thermal properties were assessed through electrochemical impedance spectroscopy (EIS) and a heat flow meter, respectively. The results were discussed and linked to micrometric porosity investigated by micro-computed tomography (μ-CT) and transport properties as determined by initial surface absorption test (ISAT), boil-water saturation method (BWS) and chloride ion penetration test. Extra-low dosage mortars, especially those loaded with a lower oxidation degree (i.e., 0.45GO), showed decreased permeability and improved barrier to chloride ion transport combined with enhanced thermal and electrical conductivity with respect to that of the control samples.