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Cellulose nanofibril (CNF) aerogels are renewable and biocompatible materials with high porosity and tunable surface chemistry. However, ultralight and ultraporous aerogels remain a great challenge to obtain high elasticity. This work focused on a scalable strategy to create large-scale lamellar-aligned CNF foam-like aerogels and the relationship between structure and mechanical properties. The morphology and mechanical properties of aerogels assembled by original TEMPOmediated oxidation CNF cross-linking with 1,2,3,4-butanetetracarboxylic acid were investigated for homogeneous freezer freezing and unidirectional gradient freezecasting. This study successfully fabricated ultralight foam-like aerogels with centimeter-sized and aligned lamellar/porous structure via cooperation of tunable chemical reaction and unidirectional gradient freezing. The resulting aerogels exhibited flyweight densities of 3−4 mg/cm 3 , enhanced recovery from 70% strain, water adsorption 82.5 times over self-weight at 20 °C and 52.0 times over self-weight at high temperature (100 °C) for 20 cycles. Moreover, the aligned aerogel followed by carbonization showed a differential and anisotropic electrical resistivity.