'Cowboys' hurdled their way to a 32-21 victory over the incumbent European champions, adding weight to their tilt to become the first men's team to win the Olympic title three times.
So far Croatia have made light work of their tough group, dismissing South Korea by 10 points, Euro 2012 runners-up Serbia by eight and Hungary by seven.
Denmark's coach Ulrik Wilbek called his side's hammering at the hands of a pumped up Croatia a "nightmare" on Saturday, with the touchline antics of his opposite number playing a big role.
"I don't think I have ever seen them play better," Wilbek told reporters, referring to the 1996 and 2004 gold medalists, who top Group B and are unbeaten.
Statistics:
Croatia 14 – 18 - 32
Debmark 9 – 12 - 21
Croatia_D.Duvnjak 5, I.Vori 5, Z.Horvat 5, B.Lackovic 3, D.Vukovic 3, D.Buntic 3, M.Strlek 3, I.Cupic 3, M.Kopljar 1, J.Gojun 1.
Denmark_A.Eggert Jensen 5, H.Lindberg 5, N.Markussen 3, M.Hansen 3, T.Mogensen 2, M.Knudsen 1, L.Svan Hansen 1, R.Toft Hansen 1.
Red Cards_None.
Referees_Nordine Lazaar, France; Laurent Reveret, France; Mansour Abdulla, Qatar; Saleh Jamaan Bamutref, Qatar; Naser Abu-Marzouq, Kuwait; Svein Olav Brudahl Oie, Norway; Alaa Elsayed Alaa, Egypt.
Earlier int he day, Croatian water polo team won Australia's 'sharks' 11-6 and sealed the unbeaten top position in their group
A penalty goal just before halftime gave Croatia a 5-2 lead at the break before four-time Olympian Thomas Whalan - who finished with a hat-trick for his first goals of the Games - scored twice to close the gap to 6-4.
'Barracudas' again pulled away as they took an 8-4 advantage into the last quarter, another goal 20 seconds into the final period sealing Australia's fate.