The attempted murder of ex-Russian spy Sergei Skripal and his daughter, Yulia, using a nerve agent was a "brazen and reckless attack", Amber Rudd has said.
Both Mr Skripal and his daughter are still critically ill after being found collapsed on a bench in Salisbury city centre on Sunday.
Counter-terrorism officers are working to find the origin of the nerve agent.
A police officer, who was in intensive care, is now "stable and conscious", Wiltshire's chief constable said.
Addressing the House of Commons, the home secretary said the attack was "attempted murder in the most cruel and public way"
Ms Rudd told MPs it was an "outrageous crime", adding that the government would "act without hesitation as the facts become clearer".
She refused to speculate on whether the Russian state might have been involved in the attack, saying the police investigation should be based on "facts, not rumour".
However, she said the government was committed to bringing the perpetrators to justice "whoever they are and wherever they may be".
A Downing Street spokesman described the attack as an "appalling and reckless crime" and said those responsible would face a "robust" response.
The fact the nerve agent is "very rare" will help the investigation narrow its focus.
Making nerve agents and delivering them requires considerable infrastructure and the more unusual the agent the easier it will be to locate which country, even which laboratory, might be involved.
That combined with police leads on who delivered the agent will form the basis for a determination of responsibility, along with any other intelligence that can be gathered.
It may take days - even weeks - for the government to be confident enough to make a public statement, because it will not want to risk getting any details wrong.
But if suspicions about Russia are confirmed, then some kind of action seems inevitable.
The legacy of the 2006 Litvinenko case shows that expelling diplomats alone may not be regarded as much of a deterrent to future acts.
Economic sanctions on the Russian elite may have more bite, but would require greater political will.
Mr Skripal, 66, was convicted of passing secrets to MI6 but was given refuge in the UK in 2010 as part of a "spy swap".
It is known that he and his 33-year-old daughter had visited the Mill pub and Zizzi restaurant in Salisbury on Sunday afternoon, before they were found collapsed on a bench near the Maltings shopping centre.
A witness, who saw the pair at the restaurant, told the BBC Mr Skripal was acting "very strange" and was "very agitated".
"He seemed to lose his temper... and he just started screaming at the top of his voice, he wanted his bill and he wanted to go."
Police have yet to say if they know how and where the poison was administered.
Defence Secretary Gavin Williamson said Russia was becoming an "ever greater threat", amid speculation the attack could have some element of state involvement.
"Russia's being assertive, Russia's being more aggressive, and we have to change the way that we deal with it because we can't be in a situation in these areas of conflict where we are being pushed around by another nation," he told ITV's Good Morning Britain.
Police said they wanted to speak to anyone who was in the centre of Salisbury on Sunday afternoon.
They are particularly keen to hear from people who ate at Zizzi or drank in the Mill pub between 13:00 and 16:00 GMT.
Both sites remain closed to the public.
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