The 70-year-old, whose final scenes as Erinsborough legend Harold Bishop screened in Australia in February, was beaten by Packed To The Rafters actress Rebecca Gibney.
Both Gibney and Smith were equal favourites with betting agency Sportingbet Australia to take the highest honour in Australian television leading up to Sunday night's ceremony.
"Thank you Tasmania, I think you got me over the line!" Gibney said in her acceptance speech. "Ian Smith had England voting for him!
"I know we sometimes pooh-pooh the Logies but this is so bloody marvellous. I'm really, really thrilled!"
Feel good family drama Packed To The Rafters was the night's big winner taking home an impressive six awards for most popular personality on television (Rebecca Gibeny), most popular actress (Rebecca Gibney), most popular new male talent (Hugh Sheridan), most popular new female talent (Jessica Marais), the Graham Kennedy award for most outstanding new talent (Jessica Marais) and most popular drama.
"This is just proof that nanas really can text. Thanks mum for spending your pension," joked Gibney on her win for most popular actress. "I wouldn't be standing here if I hadn't been given this gift of a role, so thank you."
Smash hit gangland crime series Underbelly managed to score three awards for most outstanding actor (Gyton Grantley), most outstanding actress (Kat Stewart) and most outstanding drama.
Home and Away picked up just one award with Todd Lasance taking the gong for most popular actor.
"Wow, this is awesome," Lasance said of his win. "Thank you to everyone who voted for me. I honestly wouldn't be standing here if it wasn't for you guys.
"I appreciate what I do so much. Every day I wake up I get a chance to do something that I love, go to work and work with incredible people like my cast and crew down there, and I just feel so fortunate to do what I do."
Despite receiving five nominations, including two for Ian Smith, Neighbours failed to win any accolades.