The　application　of　3D　printing　technology　in　fabricating　quasi-solid-state　micro-supercapacitors　(MSCs)　offers　inherent　benefits　in　programmable　structural　design　and　high-mass-loading　electrode　fabrication.　Nevertheless,　the　absence　of　high-performance　printable　inks　and　the　sluggish　ion　transport　within　thick　electrodes　present　significant　challenges　to　their　practical　charge　storage　capabilities.　Here,　a　new　NiCo2S4-based　nanocomposite　ink　with　excellent　rheological　properties　has　been　successfully　developed　and　the　3D　structure　of　quasi-solid-state　MSCs　is　rationally　engineered　through　the　direct-ink-writing　3D　printing　technology.　Beneficial　from　the　firmly　anchored　NiCo2S4　nanoparticles　on　the　reduced　graphene　oxide　(rGO)　and　the　ordered　3D　micropores,　the　thick　electrodes　with　serrated　architectures　provide　abundant　reaction　sites　and　exhibit　enhanced　ion　transport.　Consequently,　the　MSCs　with　triple-layer-serrated　electrodes　can　deliver　a　high　areal　capacitance　up　to　416.7　mF　cm(-2).　In　comparison　to　the　latticed　counterparts,　the　areal　capacitances　of　serrated　MSCs　with　single-,　double-,　and　triple-layer　electrodes　are　amplified　by　127.1%,　349.8%,　and　585.9%,　respectively　(under　1　mA　cm(-2)).　This　study　offers　novel　insights　into　the　cross-scale　design　of　materials　and　electrode　architectures　for　quasi-solid-state　MSCs　with　high　areal　capacitance,　promoting　their　integration　into　flexible　and　portable　electronic　devices.