The 3D freeze printing (3DFP) of nanocellulose aerogels are demonstrated with large-scale aligned pore orientations as a sustainable alternative to current acoustical materials. In contrast with the unidirectional pore network orientations obtained from current 3DFP techniques, a bidirectional orientation is achieved by using an inhomogeneous printing substrate to alter the thermal gradient within the print volume. The microstructural morphology shows that bidirectional printing results in a 2D pore orientation, with comparatively thinner pore walls and larger pore widths. Acoustic measurements reveal that altering the pore network characteristics significantly affects the acoustical behavior of the printed CNC aerogels; the wider pores allow the bidirectional CNC aerogels to provide higher sound absorption performance at lower frequencies than the unidirectional samples. Notably, both 3D Freeze printed CNC aerogels provide substantially higher sound transmission loss performance as compared to current acoustical materials. The unidirectional pore structure results in CNC aerogels with higher stiffness and improved energy absorption performance, with both 3D freeze printed CNC aerogels outperforming other CNC aerogel materials in their stiffness-to-density ratios. The ability to simultaneously control their pore orientation and macrostructural geometry paves the way for printing complex shaped CNC aerogel structures for multifunctional noise control applications.