Thin-felt NiO-Al2O3/FeCrAl-fiber catalysts engineered from micro- to macro-scales are developed for the high-throughput catalytic oxy-methane reforming to syngas. Crystallization-driven self-assembly process is used to prepare an Al(OH)3/FeCrAl-fiber support (15wt% Al(OH)3). NiO of ~3wt% is then highly dispersed onto above support via incipient wetness impregnation method followed by a calcination treatment. Such catalyst achieves a high CH4 conversion of 88.6% with 90.7%/93.2% selectivity to H2/CO at 700°C and a high gas hourly space velocity of 80Lg−1h−1, and is stable for at least 30h without carbon deposit but a slight sintering. In contrast, a reference catalyst of NiO/FeCrAl-fiber shows a fast deactivation within only 6h.