Realizing　MoS2　basal　plane　activation　is　highly　desirable　and　challenging　in　the　field　of　hydrodesulfurization　(HDS).　Herein,　we　have　developed　a　new　strategy　of　dual　Co　single　atom　doping　(SAD)　combined　with　CO　in　situ　regulation,　which　can　successfully　activate　the　basal　plane　of　Co-3.6%-MoS2-0.3　generating　high　ratios　of　thermostable　1T-plane　(similar　to　70%)　and　large　S　vacancies.　For　the　first　time,　a　synergistic　effect　has　been　unraveled　where　the　lattice　substituted　neighboring　dual　SA　Co　can　efficiently　activate　in-plane　S　through　extensively　reducing　its　band　gap　(2.21　-＞　0.14　eV),　which　tremendously　favors　S　subtraction　and　2H　-＞　1T　phase　transition　assisted　by　CO.　Boosted　thiophene　HDS　activity　can　be　eventually　achieved　with　the　reaction　rate　constant　(k)　being　8.3　times　higher　than　that　of　commercial　(c)　Co-3.6%-MoS2　(0.04　-＞　0.33　h(-1)).　Generally,　the　present　work　paves　a　new　way　for　next-generation　HDS　catalyst　design　with　activated　basal　plane.