“…This particularly holds when they are internally ordered and exhibit reasonable mechanical strength as individual sheet entities and thus, qualify as "2D Polymers" (2DPs). [ 2 ] Fields of applications that one can envisage [ 3 ] include chiral surfaces, [ 4 ] molecular electronics, [ 5,6 ] nanopatterning, [ 7 ] molecular landscaping, [ 8 ] acoustic sources, [ 9 ] chemiresistors, [ 10 ] nano-sieves, [ 11 ] hierarchical interactions, [ 12 ] stem-cell regulation, [ 13 ] phonontransport, [ 14 ] and molecular machines.[ 15 ] Ever since the fi rst polymerization experiments were conducted to obtain ultrathin fi lms at the air/water interface in 1930s, [ 16 ] numerous attempts were reported to create covalent monolayer sheets [ 1,[17][18][19][20] at air/ liquid and liquid/liquid interfaces as well as on solid substrates. While they led to intriguing developments and invaluable insights into the problems associated with approaching such synthetic targets, a key aspect remained unravelled: the longrange covalent order in the obtained sheets.…”