The American threw her hands in the air, shook her head, gesticulated towards her coach and stomped her feet in petulant protest - but that did little to help compatriot Varvara Lepchenko who suffered a 6-2 6-1 first round defeat.
Howling with frustration in her first match since winning the WTA Championships at Istanbul in October, lacking rhythm in swirling winds on Pat Rafter Arena, Williams still delivered enough booming serves and punishing groundstrokes to prevail in a formidable if cantankerous display.
The reigning Wimbledon, Olympic and U.S. Open champion told reporters a calendar-year grand slam was very much on her mind at the start of the season.
Williams held all four major titles in the so-called Serena Slam of 2002-2003 but the holy grail of professional tennis is to win the Australian Open, French Open, Wimbledon and U.S. Open tournaments in the same calendar year.
The American claimed world number one Victoria Azarenka and number two Maria Sharapova, and perhaps a few fringe-dwellers, were eyeing off a near-impossible feat not achieved since Steffi Graf's unbeaten run through 1988.
"I think whoever wins the Australian Open will have that same thought," Williams said.
"I think there is no way that Victoria or Maria or maybe some other players don't have that same thought. I think I definitely feel that way."
Both Azarenka and Sharapova are in a red-hot Brisbane field with Williams. Of the world's top 10, only Agnieszka Radwanska and Li Na are missing.
The predictability of her defeat of Lepchenko was matched by the level of emotion surrounding Australian wildcard Jarmila Gajdosova's victory on the opening day.
Playing her first tournament since the passing in September of her mother, also named Jarmila, and with her world ranking having plummeted from a career high of 25 to 183 in the last 18 months, Gajdosova roared home from a one-set deficit to stun Italy's world number 16 Roberta Vinci.
Gajdosova wept after a 4-6 6-1 6-3 triumph that set up a second-round showdown against French Open champion Sharapova.
"There have been a lot of things happening in my life," Gajdosova said.
"As you all know, my mom passed away in September. It's been a difficult time. First Christmas, as well, without her. My dad is here. My brother and his wife and son. It was my first match in front of them and my first match in Australia, after a long time, without my mum."
Sixth-seeded Czech Petra Kvitova recovered from a pre-tournament asthma scare to defeat Spain's Carla Suarez-Navarro 6-3 6-4.
Kvitova has been gasping and wheezing in Brisbane's humid weather and revealed one of her recent attacks had been her worst in three years.
The 2011 Wimbledon champion was unaware she was asthmatic until she nearly collapsed during an event in New York in 2009.
"I was playing a tournament in the Bronx and after about five minutes I had to sit down and relax and have a drink because I just couldn't move and I couldn't play," she wrote in a column for the Courier-Mail newspaper.
"I still feel really uncomfortable when I'm in this sort of hot and humid weather and it was at practise on Friday that I started to feel a bit similar to what I did in The Bronx."
First-round results, WTA Brisbane
3-Serena Williams (U.S.) beat Varvara Lepchenko (U.S.) 6-2 6-1
6-Petra Kvitova (Czech Republic) beat Carla Suarez Navarro (Spain) 6-3 6-4
Daniela Hantuchova (Slovakia) beat Lourdes Dominguez Lino (Spain) 7-5 6-2
Anastasia Pavlyuchenkova (Russia) beat Lucie Hradecka (Czech Republic) 6-3 3-6 6-3
Jarmila Gajdosova (Australia) beat Roberta Vinci (Italy) 4-6 6-1 6-3
Urszula Radwanska (Poland) beat Tamira Paszek (Austria) 2-6 6-0 6-2