Eitam and Naama Henkin, both in their 30s, were gunned down while driving on Thursday night between the settlements of Itamar and Elon More, in the north of the Palestinian territory.
Their four children, aged between four months and nine years, were found unharmed in the back of the car.
Israeli army spokesman Arye Shalicar said security forces were conducting an "intensive search" on the ground combined with intelligence efforts.
The Henkins were residents of the central West Bank settlement Neria, northwest of Ramallah. They were to be buried in Jerusalem's Har Hamenuhot cemetary at 0800 GMT on Friday.
In the Palestinian village of Beitillu, a short distance from Neria, assailants torched a car and spray-painted "Revenge Henkin" on a nearby wall, the army said on Friday, noting that nobody was hurt.
Apprehensive of rising tensions among settlers and Palestinians, the army said it would be deploying "four battalions in order to prevent an escalation of violence in the area adjacent to the location of the attack."
Thursday's shooting came hours after Prime Minister Benjamin Netanyahu's address to the United Nations General Assembly, and a day after that of Palestinian president Mahmud Abbas, who said that Israel's refusal to release prisoners and stop settlement activity was hampering fresh peace talks.
Netanyahu condemned the killings, which he called "the effects of Palestinian incitement," vowing security services would work to "capture the murderers and improve security for all Israeli citizens."
- 'Crimes of the Zionists' -
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Tensions have been running high between Israeli police and Palestinians at the Al-Aqsa mosque compound in Jerusalem.
The site of Thursday's shooting was near the Palestinian village Beit Furik, where a Palestinian was killed by Israeli forces during clashes last month.
Israeli Defence Minister Moshe Yaalon said security forces would "spare no efforts to arrest the killers and their sponsors".
The Palestinian militant group Hamas for its part hailed those behind Thursday's deadly attack, while not taking responsibility for it.
"This operation was in response to the crimes of the Zionists," it said in a statement.
Israel occupied the West Bank in the 1967 Six-Day War in a move never recognised by the international community.
Hardline Jewish nationalists see the entire West Bank as part of Israel, which refers to the territory as Judea and Samaria, the names for the ancient biblical kingdoms located there.
The last killing of an Israeli in the West Bank happened on June 29 when a settler died and three others in a car with him were wounded.
On July 31, suspected Jewish extremists firebombed a Palestinian home in the village of Duma that killed toddler Ali Saad Dawabsha and his parents.