....with a collection of his earliest appearances (as well as a couple of extras) from 100-Page Super Spectacular #DC-20 from September, 1973, all under a cover by Nick Cardy.
Detective Comics #66
This is when we see District Attorney Harvey Kent take acid to the face as he was prosecuting Boss Maroni, scarring half his face, making Kent use Maroni's two-headed coin (with one side now scarred as well) to make decisions, with the clean side representing good, and the scarred, evil. Batman feels it is his responsibility to catch and rehabilitate Two-Face, but Two-Face is undecided, with his coin landing on its edge when he was deciding whether to be a hero or villain.
Detective Comics #68
Putting the coin in his pocket, it is the coin that saves Two-Face when a cop shoots him in an attempt to stop the ex-attorney, making Two-Face lean to evil. Two-Face begins crimes focused on the number two, and tries unsuccessfully to reconcile with his fiancee, Gilda, hiding half his face with help from a make-up artist (which eventually fails, leading Two-Face into a vendetta with the artist, and the artist's son to want revenge on Two-Face). Batman stops this series of events.
All-American Comics #88
Thankfully, Dr. Mid-Nite was able to blackout Tarantula's suspicions....
Flash Comics #95
Investigating as Black Canary, she ends up at the home of Andrew Masters, who has been murdered...and Black Canary has been framed! Turns out Masters' niece committed the crime and the frame, because Masters changed his will to leave his money to Black Canary.
Adventure Comics #66
Starman (Ted Knight) faces off against Cuthbert Cain, who uses a special camera powered by voodoo magic to steal men's souls, who takes a picture of FBI agent, Woodley Allen, to keep him from interfering with Cain's plans.
Starman turns the tables on Cain using his own Gravity Rod, using Cain's camera on him, making Cain disappear and breaking Cain's hold on Allen....
The lady Fear gets help from Starra, who has managed to control a small European country by marrying it's prince, Ghor, to face off against Blackhawk and his men, but it doesn't end well for Starra, being killed by Fear as Starra was not able to manipulate Fear as well as she did her husband.
Fear also realizes how strong her feeling are for Blackhawk...
More Fun Comics #66
This time, Spectre has to stop giant creatures who are menacing his home of Cliffland, but he is surprisingly weakened by their green eyes. Spectre follows the creatures to a museum, where he learns their secret...that they live within the paintings!
After destroying the painting that housed the monsters, the Spectre saves his girlfriend, Clarice Winston, from criminals who were menacing her.
Sensation Comics #71
This story features a battle between Wildcat and his foe, the Huntress, as she tries to hurt Ted by kidnapping Wildcat's assistant, Stretch Skinner, so that Ted will have to miss a championship fight.
Wildcat is able to free Stretch from the Huntress, then take out the imposter Huntress had replacing Ted Grant in the ring.
Detective Comics #80
Harvey escapes prison to go on a criminal rampage, but accidentally shoots his fiancee, Gilda, during his spree.
This causes Harvey to want to reform, helping Batman defeat his gang, and Batman gets a doctor to perform plastic surgery on Two-Face, theoretically ending the menace of Two-Face forever (or at least until Batman #50 of 1948, but that's another tale...).