An alleged crime spree, including two home invasions on Sydney's north shore and three police chases, has ended in the death of two men on their way to work.

Earlier this week, homes in Mosman and Lavender Bay were broken into in the middle of the night as the occupants were asleep inside.

A Toyota Hilux ute was stolen from one of the properties.

In the early hours of Thursday morning, the mangled remains of that grey four-wheel-drive ute were strewn across an intersection at St Peters in Sydney's inner west.

Moments earlier, just after 4.30am, the stolen ute, with 33-year-old Raymond Lomas allegedly behind the wheel, slammed into a Hyundai sedan on the Princes Highway, killing two people.

The victims, a 62-year-old man and 49-year-old man, were driving towards Silverwater, where they were due to start early shifts at a printing company.

The double fatality came after Mr Lomas allegedly tore a reckless path across the city, stretching from Waterloo to the inner-west suburbs.

Police, who were on the lookout for the stolen car, pursued the ute in Waterloo on Thursday morning but called the chase off when it became too dangerous.

One motorist said the ute "almost took me out" when it sped past him, with a police car in tow.

"I stopped my car and noticed 10 police cars giving chase. It started near Waterloo. Devastating news to hear how it's ended," he said.

The ute was then seen driving down the wrong side of the Princes Highway near Sydenham.

It crashed into a car near Railway Road, allegedly injuring a man before continuing down the highway.

The ute then allegedly sped through a red light at the intersection of Princes Highway and Canal Road at St Peters in full view of a stopped police car.

It then crashed into the Hyundai, killing both men inside.

A police dog squad car was waiting at the traffic lights across the road and saw the crash unfold. The officer jumped out of the car to arrest Mr Lomas, from Waterloo, as he tried to flee.

"The driver of the stolen vehicle sustained injuries to his leg as a result of the arrest by the dog squad officer," NSW Police acting Assistant Commissioner Michael Fitzgerald said.

"He is currently in hospital where he will be later interviewed by police in relation to this incident."

Police say while the driver was involved in police pursuits earlier in the morning, the last chase was called off 10 minutes before the fatal smash.

"That vehicle entered into three pursuits at about 4am, 4.15am and 10 minutes prior to the incident," Mr Fitzgerald said.

"At the time, and I want to make this very clear, police were not actively involved in a pursuit of that vehicle when it collided with the car carrying the two vicitms."

A critical incident investigation will now carefully look at the police actions leading up to the double fatality.